Open Access Article
Gang Huang†
ab,
Ruosi Chen†
c,
Mingxi Chen†
d,
Xianfeng Chen
bd,
Mengting Jiang
d,
Yu Xing
b,
Jiang Wangd,
Boqun Liang
e,
Qiushi Liu
f,
Xiangdong Li
g,
Chit Siong Lau
bd,
Xiaonan Dong
hi,
Piyush Agarwald,
Lin Ked,
Syed M Assad
bd,
Jian-Rui Soh
bd,
James Lourembam
d,
Young-Wook Cho
bd,
Qingcheng Liang
*a,
Jian Li
*j,
Xiao Zhang
*k,
Yuan Ma
*k,
Yuerui Lu
*c,
Ping Koy Lam
*bd and
Xuezhi Ma
*bd
aSchool of Materials Science and Engineering, Changchun University of Science and Technology, Changchun, 130022, China. E-mail: liangqingcheng@cust.edu.cn
bQuantum Innovation Centre (Q. InC), Agency for Science, Technology and Research (A*STAR), 4 Fusionopolis Way, Kinesis, #05, Singapore, 138635, Republic of Singapore. E-mail: pingkoy@a-star.edu.sg; ma_xuezhi@a-star.edu.sg
cSchool of Engineering, College of Engineering and Computer Science, The Australian National University, Canberra, Australian Capital Territory 2601, Australia. E-mail: yuerui.lu@anu.edu.au
dInstitute of Materials Research and Engineering (IMRE), Agency for Science, Technology and Research (A*STAR), 2 Fusionopolis Way, Innovis, #08-03, Singapore 138634, Republic of Singapore
eMaterials Science and Engineering program, University of California-Riverside, Riverside, California 92521, United States
fShanghai Institute of Optics and Fine Mechanics, Chinese Academy of Sciences, Shanghai, 201800, China
gGuangzhou Wide Bandgap Semiconductor Innovation Center, Guangzhou Institute of Technology, Xidian University, Guangzhou 510555, China
hLife and Health Institute, China Resources Research Institute of Science and Technology Company Ltd, Hong Kong S.A.R., China
iSchool of Biomedical Sciences, LSK Faculty of Medicine, the University of Hong Kong, Hong Kong S.A.R., China
jState Key Lab of Analytical Chemistry for Life Science, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing 210023, China. E-mail: jianli@nju.edu.cn
kDepartment of Mechanical Engineering, The Hong Kong Polytechnic University, Hong Kong 999077, China. E-mail: xiao1.zhang@polyu.edu.hk; y.ma@polyu.edu.hk
First published on 6th January 2026
The field of two-dimensional (2D) materials has seen remarkable progress, driven by their exceptional electronic, optical, and mechanical properties. In addition to their intrinsic qualities, 2D materials are atomically thin and readily integrated with a wide range of devices, offering immense potential for next-generation on-chip technologies across various domains, beyond just electronics and optics. Central to the fabrication of 2D devices is the development of effective transfer methods, which are crucial for maintaining clean material interfaces and intact material properties. However, as some of the most fundamental techniques, transfer methods are incredibly diverse, making it challenging to navigate the various approaches. This review provides a comprehensive analysis of the state-of-the-art transfer methods, including a preliminary discussion on high-quality 2D material preparation, along with evaluation of the strengths and weaknesses of various transfer techniques. Furthermore, despite being a foundational field, there are still many significant tasks to be undertaken, with several bottlenecks awaiting breakthroughs. We also highlight emerging trends, such as reconfigurable transfer, all-transfer for chip manufacturing, and the application of transfer techniques to low-dimensional materials across broader research fields, such as chemistry, polariton, tribology, haptics, thermal transport, thermodynamic control, quantum science, neuromorphic computing, electrocatalysts, and energy, offering insights into future directions for 2D material integration.
To achieve high-performance 2D devices, it is essential to maintain both the intrinsic quality of the 2D materials and the cleanliness and flatness of their interfaces throughout the entire fabrication process. This involves two primary challenges: (1) producing high-quality, wafer-scale 2D films and flakes and (2) integrating them with various device platforms.
Two main approaches exist for producing 2D materials: top-down exfoliation and bottom-up growth. Top-down methods, such as mechanical exfoliation,9,10 electrochemical delamination,11 and liquid-phase exfoliation,12 offer excellent material quality but are often limited by sample size and scalability. In contrast, bottom-up methods, including physical vapor deposition (PVD) and chemical vapor deposition (CVD),13,14 offer better scalability but face challenges like uncontrolled nucleation, grain boundary formation, and lattice mismatch, which can degrade film quality.15 Regardless of the approach, the ultimate goal remains the same: to produce large-scale 2D films with high crystallinity, low defect densities, and excellent transferability, enabling their seamless integration into wafer-scale devices. Achieving this goal requires not only precise control over the growth or exfoliation process but also innovative transfer techniques that preserve the chemical and structural integrity of the 2D materials.16
As 2D materials transition from fundamental research to practical applications,17–19 the ability to precisely transfer these atomic-scale layers onto diverse substrates becomes increasingly critical. Effective transfer methods are essential for integrating 2D materials into complex heterostructures, minimizing contamination and preserving exceptional intrinsic properties, all of which are crucial for high-performance electronic, photonic, and quantum devices.
Earlier transfer approaches for building heterojunctions primarily relied on polymer supports, such as polymethyl methacrylate (PMMA). However, these methods often trap contaminants at the interfaces of 2D materials, diminishing the advantages of their unique properties. To overcome these limitations, dry methods such as the clean polydimethylsiloxane (PDMS) stamp method and capillary force assisted methods have been developed, offering improved interface cleanliness and more feasible protocols. After more than ten years of development, transfer methods have been optimized for different application scenarios. However, none of the current transfer methods are perfect and cannot accommodate all requirements at once. Our goal is therefore to provide a comprehensive review that will serve as a guide for entry-level researchers to get them started quickly and to recommend transfer methods that guarantee high in-plane and out-of-plane quality of 2D materials, while also being easy to use, depending on the application scenario. Additionally, considering that many research groups have their routinely used methods, we aim to introduce some advanced techniques, such as silicon nitride (SiNx) membrane clean transfer,20 ultraviolet (UV) tape wafer-scale transfer,21 and graphene-mediated single-crystal oxide transfer,22 to experts who typically rely on established techniques.
Beyond the fundamental role of transfer in integrating 2D materials into devices, these processes can also unlock unique physical phenomena by intentionally or unintentionally introducing structural deformations. These deformations, such as bending, twisting, and wrinkling, can serve as powerful tools for manipulating the electronic, optical, and mechanical properties of 2D materials, offering new avenues for device design and fundamental research.
In addition to reviewing established methods, we will explore emerging techniques such as reconfigurable transfer methods and the all-transfer approach for wafer-scale chip fabrication. Most of the currently available transfer methods focus on building a stack of 2D materials like building “LEGO” blocks.23 However, a true “LEGO” functionality should also allow for disassembly and reassembly. Reconfigurable transfer methods, which enable the assembly, disassembly, and reassembly of 2D structures, offer a promising direction for exciting applications, such as the “control variable method” at the nanoscale. Moreover, the role of transfer methods in the manufacturing of future electrical and optical devices could expand significantly through all-transfer approaches.
The all-transfer strategy, wherein every device component—from active 2D semiconductors to electrodes, dielectrics, and even complete device stacks—is assembled by transfer rather than direct fabrication, marking a paradigm shift in 2D electronics. By eliminating lithography and harsh processing, it preserves intrinsic material quality, ensures pristine interfaces free from disorder and Fermi-level pinning, and enables scalable, low-cost, and high-performance device integration—offering a transformative route toward industrial adoption of 2D materials.
Finally, we have observed that transfer methods are already being applied in a variety of broader fields, such as in chemistry,24 polaritonic devices,25 phonon polaritons,26 tribology,27 haptics,28 thermal transport,29,30 thermodynamic control,31 quantum devices,8 neuromorphic computing,32 electrocatalysts and energy.33,34 We believe that transfer techniques will continue to play a significant role across many scientific disciplines, offering versatile solutions and broadening their impact in diverse areas of research and technology.
In summary, this review will provide a comprehensive summary on emerging transfer methods for 2D device fabrication. It begins with the preparation of 2D materials, focusing on wafer-scale approaches as a foundation for transfer techniques. We then provide a comprehensive assessment of transfer methods, including dry, wet, capillary force assisted, and emerging strategies such as UV tape-assisted and SiNx membrane techniques. A radar chart is used to visualize and compare nine representative methods across multiple performance metrics. This section also covers the transfer of 2D and low-dimensional materials on arbitrary substrates, enabling diverse photonic and electronic integrations. In the third section, we explore multifunctionalities made possible by transfer techniques, such as strain, wrinkle, bubble, fold, and twist engineering—which unlock novel properties and device concepts. The perspective section highlights reconfigurable and all-transfer approaches as promising directions for next-generation device manufacturing. Finally, we reflect on the broader impact of transfer methods in fields such as chemistry, wearable electronics, quantum optics, and mechanics, offering insights into their transformative potential.
The quality and transfer readiness of 2D materials are strongly influenced by both interfacial chemistry, which governs the bonding between layers or between the film and its growth substrate, and surface chemistry, which determines terminal functional groups, surface charge, and defect states. For example, modifying interlayer bonding through ion or molecule intercalation can reduce exfoliation energy, while controlling surface terminations can improve compatibility with downstream processing. Furthermore, the interaction strength between the 2D layer and its substrate, shaped during synthesis, critically affects subsequent transfer efficiency, yield, and cleanliness.
This section therefore outlines the essential principles and representative examples of each preparation route, while highlighting the interplay between growth chemistry, interfacial engineering, and substrate interactions that ultimately dictate transfer performance in device fabrication.
Effective exfoliation requires precise control over both interfacial chemistries, modifying interlayer bonding, often through ion or molecular intercalation, to reduce exfoliation energy and enhance layer separation and surface chemistry, which governs terminal functional groups, surface charge, and defect states, thereby influencing reactivity and compatibility with downstream device processing.
Traditional mechanical exfoliation offers simplicity and is typically performed by peeling 2D materials from high-quality layered crystals using an adhesion layer.40,41 However, this method lacks precise control over the cleavage environment.42 Issues such as random fracture and limited transferable area often arise due to non-conformal contact between the adhesion layer and the 2D material, uneven decoupling between the growth substrate and the 2D material, and uncontrolled bending stress.43 For example, in 2015, Sutte, Huang et al. adopted plasma pretreatment to improve the stripping efficiency and size of 2D materials (Fig. 1a).44 Before exfoliation, they used oxygen plasma to clean the contaminants adsorbed on the substrate from the environment to increase the adhesion between the substrate and the 2D material, and through thermal treatment, they maximized the contact area between the bulk crystals and the substrate.39 While this method provides an effective way to exfoliate the high quality and relatively large size 2D flakes (several hundred micrometres),45 it cannot be easily applied to wafer scale exfoliation.
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| Fig. 1 Exfoliation of 2D materials. (a) Large size 2D material flake exfoliation method enabled by an oxygen plasma cleaned substrate. Reproduced from ref. 44 with permission from American Chemical Society, Copyright 2015. (b) Large area 2D material flake exfoliation by electrochemical methods. Reproduced from ref. 11 with permission from American Chemical Society, Copyright 2011. (c) Metal-assisted exfoliation method. Large flakes of 2D materials can be achieved (I–III). More interestingly, this method also enables the exfoliation with patterning (IV–IX). Adapted from ref. 39 according to Creative Commons Attribution 4.0 International License (CC BY 4.0). Reproduced from ref. 62 with permission from Wiley-VCH, Copyright 2016. Reproduced from ref. 56 with permission from Wiley-VCH, Copyright 2024. | ||
To achieve larger flakes, emerging exfoliation methods, such as electrochemical exfoliation46–49 and supercritical fluid exfoliation,50–52 provide more precise chemical control by tuning thermodynamic (e.g., electrode potential and solvation energy) and kinetic (e.g., ion migration rate and solvent diffusion) parameters. These methods enable the introduction of specific surface groups or defect states, facilitating more customized material design for electronic, optoelectronic, and quantum device applications.
Liquid-phase exfoliation disperses bulk crystals in solution and induces delamination through either physical (e.g., ultrasonication) or chemical (e.g., electrochemical reactions) methods. While ultrasound can effectively separate layered materials, the violent cavitation bubbles it generates often fracture or degrade the nanosheets, compromising their structural integrity and electronic quality.53 By contrast, electrochemical exfoliation offers tunable control via applied current and cutoff voltage, enabling a more deterministic process. Yet, the bubble-driven reactions readily oxidize and consume copper electrodes, hindering their recyclability and long-term scalability. This intrinsic limitation poses a significant barrier to the broader industrial deployment of electrochemical exfoliation (Fig. 1b).11
The metal-assisted exfoliation method is a more efficient exfoliation technique that can yield large flakes (Fig. 1c, Scheme and I–III). It does not require polymer materials as adhesives, thus avoiding the residue of polymers on the surface of 2D materials. Moreover, the metal film has greater mechanical strength and can better protect 2D materials from wrinkling or cracking. Since the development of the Cu-assisted transfer method by Lin et al. for the successful transfer of centimeter-sized MoS2 films,54 researchers have developed various metal-assisted exfoliation methods, such as Ni,55 Au,56 Ag,57 etc.
Au-assisted exfoliation, one representative of metal-assisted approaches, has emerged as a promising strategy for obtaining large-area monolayer TMDCs, owing to the strong adhesive force between gold and 2D flakes.58,59 However, the effectiveness of this method is highly dependent on the surface roughness of the gold film, which in turn is determined by the underlying deposition substrate.60 To better understand the mechanism behind Au-assisted exfoliation, researchers conducted first-principles studies comparing the binding energies of Au–MoS2 and MoS2–MoS2 interfaces.61 It was revealed that the Au–MoS2 interaction is governed by strong vdW forces rather than true chemical bonding. The role of gold surface roughness was also systematically investigated, showing its critical impact on exfoliation efficiency. Up to now, innovations such as a thermal release tape (TRT) tape have significantly enhanced the success of Au-assisted exfoliation, enabling the verified isolation of over 40 types of 2D materials.39,62
One of the most notable aspects of the Au-assisted exfoliation method is its ability to combine patterning with exfoliation, as demonstrated by Bao et al. through an Au template-assisted mechanical exfoliation strategy (Fig. 1c(IV)–(IX)).56 This technique enables the production of atomically thin, large area 2D crystals while avoiding contamination associated with wet chemical processes. Additionally, it addresses the limitations of traditional dry transfer, such as the restricted variety and small size of materials. In addition to gold, silver has also been explored as an intermediate layer for large-area exfoliation of 2D semiconductors.57 Both gold and silver are currently the most reliable auxiliary materials for assisted exfoliation. However, their high cost remains a major barrier to widespread commercial adoption.
Recently, techniques including sputtering, molecular beam epitaxy (MBE), atomic layer deposition (ALD), pulsed laser deposition (PLD), and vapor-phase deposition methods, such as CVD, PVD, and metal–organic CVD (MOCVD), have been developed and optimized to bridge the gap between laboratory research and practical applications of 2D materials (Fig. 3a–d). To provide a more intuitive overview, we also present in Fig. 2, a roadmap of the development of 2D material growth techniques, highlighting both their historical evolution and emerging trends. These advancements also lay a solid foundation for further studies on 2D material transfer.63 Epitaxial growth, a key synthesis strategy, enables atomic or molecular assembly of 2D materials on diverse substrates. Combined with the above preparation techniques, it allows precise control over composition and crystallinity, offering significant potential for producing high-quality, single-crystal, and wafer-scale 2D films.64,65
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| Fig. 3 Growth of 2D materials. (a)–(d) Schematic of 2D material growth techniques by MBE, ALD, PLD, and CVD, respectively. (e) Surface nucleation mechanism of graphene on a Cu substrate. Reproduced from ref. 67 with permission from Springer Nature, Copyright 2024. (f) Growth mechanism of the proposed hypotaxy. Reproduced from ref. 70 with permission from Springer Nature, Copyright 2025. (g) Patterned single crystal 2D material growth via geometric confinement. Reproduced from ref. 71 with permission from Springer Nature, Copyright 2023. (h) Low-temperature growth by MOCVD. Reproduced from ref. 72 with permission from Springer Nature, Copyright 2023. (i) Schematic of vdW epitaxy of TMDCs on a sapphire substrate. (j) Dual-coupling-guided epitaxial growth mechanism of WS2 on a two-inch sapphire wafer. Reproduced from ref. 73 with permission from Springer Nature, Copyright 2021. (k) Layer-by-layer and 3D-island growth of multilayer 2D materials. (l) Schematic of controlled growth for out-of-plane and in-plane heterostructures. Reproduced from ref. 74 with permission from American Chemical Society, Copyright 2022. | ||
Nucleation commonly occurs at high-energy sites on the surface, such as steps, twists, defects, scratches, and nanoparticles on the substrate. Seeding promoters are commonly used to artificially facilitate the nucleation process. For instance, the substrate modified by reduced graphene oxide (rGO) or perylene-3,4,9,10-tetracarboxylic acid tetrapotassium salt (PTAS) can significantly improve crystallinity, uniformity, and controllability.69 Recently, Moon et al. demonstrated the “hypotaxy method” by using graphene templates to precisely regulate MoS2 nucleation and thickness (Fig. 2f).70 This approach enabled the fabrication of wafer-scale, single-crystal MoS2 layers with high thermal conductivity (∼120 W m−1 K−1) and mobility (∼87 cm2 V−1 s−1).
Another approach to controlling nucleation is pre-patterning the substrate to directly obtain patterned 2D materials, thereby eliminating the need for photolithography and etching processes.71,75–78 For example, Kim and colleagues achieved the growth of single-domain arrays by geometric confinement, adjusting the difference in surface binding energy within the patterned SiO2 array and confining nucleation to the target area (Fig. 3g).71,75 By optimizing the array size, they fabricated single-domain arrays with excellent electrical performance, reliably avoiding grain boundaries and the introduction of defects caused by etching post-processing.
Beyond substrate pre-patterning strategies, another widely adopted approach involves the use of low-melting-point precursors, such as metal halides and metal–organic compounds, or molten-salt-assisted processes.79–81 In pursuit of compatibility with complementary metal-oxide-semiconductor (CMOS) back-end-of-line integration, the semiconductor industry has been striving to confine the growth temperature of 2D materials below 450 °C, a threshold that would substantially accelerate their industrial deployment. Compared with metal oxide precursors, low-melting-point species can generate a higher vapor flux, promote precursor diffusion and facilitate the nucleation of 2D layers at low temperature.82
Notable work includes the use of (NH4)2MoS4 or metal iodides to achieve the low-temperature, large-area growth of 2D materials.83,84 Moreover, organometallic precursors such as Bi(C6H5)3 and (CH3)2Se2 have enabled the synthesis of Bi2O2Se thin films at 300–400 °C, dramatically lowering the temperature from conventional values near 1000 °C.85 Zhu et al. employed Mo(CO)6 as a volatile precursor to realize monolayer MoS2 growth below 300 °C within 60 min, directly on silicon-based CMOS circuits.86 More recently, Hoang et al. further utilized the same precursor to achieve the direct synthesis of a high-crystalline MoS2 monolayer at temperatures as low as ∼150 °C, setting a new record for low-temperature growth and even enabling deposition on flexible polymer substrates (Fig. 3h).72 In addition, ALD has emerged as a versatile low-temperature technique, offering atomically precise thickness control through self-limiting surface reactions.87 Recent studies have demonstrated that ALD enables the conformal growth of ultrathin, high-κ dielectrics, such as sub-3 nm Al2O3 and HfO2 films on 2D surfaces, greatly improving interface quality and gate controllability in MoS2 transistors.88,89 This breakthrough demonstrates excellent CMOS compatibility and potential for wearable electronics, although the polycrystalline MoS2 films produced at such low temperatures still require further optimization to meet the mobility standards specified by the International Roadmap for Devices and Systems (IRDS) roadmap.90,91
For example, high-quality graphene and h-BN have been widely reported to be grown on transition metal substrates like Cu and Ni using techniques such as CVD and MBE, or through epitaxial graphitization on the top surface of hexagonal SiC crystals.95–99 In this case, transition metals act as both the growth substrate and the catalyst for hydrocarbons or borohydrides. Notably, graphene and h-BN share the same lattice structure and have closely matched lattice constants. A large number of experimental observations and theoretical predictions are consistent, showing that they have the maximum binding energy along the Cu(110) direction and tend to grow on Cu(111) and Cu(110). Especially, Cu, due to its very low carbon solubility, is considered an ideal substrate for the preparation of large-scale, high-quality, and uniform monolayer graphene or h-BN. However, graphene has C6v symmetry, while h-BN has lower C3v symmetry, which results in the formation of twin boundaries when h-BN 2D domains merge, making it more difficult to generate single-crystal films.64,100
Unlike graphene, the growth of TMDCs does not require catalytic substrates, instead, Cu or Ni substrates tend to undergo sulfidation. The chemically inert graphene layer and Au film have become the suitable template for epitaxial growth. Shi et al. and Gao et al. demonstrated the epitaxial growth of MoS2 on CVD-grown graphene and WSe2 and Au(111) surfaces, respectively.101,102 In recent years, researchers have successfully synthesized wafer-sized TMDC single crystals on sapphire substrates. Various methods, such as sulfur-rich conditions, substrate annealing for atomic smoothness, and Ni foam, have been used to adjust the orientation of 2D domains.103–105 However, the low symmetry of h-BN and TMDCs leads to inverse parallel domains, forming twin boundaries that significantly degrade their electronic properties. To solve this challenge, Wang et al. achieved the epitaxial growth of a 10 × 10 cm2 single-crystal h-BN monolayer on a Cu(110) vicinal surface. By step-edge coupling between the Cu(211) step and h-BN zigzag edges, they attained unidirectional orientation exceeding 99% and proposed the concept of “step-edge guiding epitaxy”.106 Yang et al., in 2020, achieved wafer-scale epitaxial growth of single-crystal MoS2 monolayers on vicinal Au(111) thin films by melting and resolidifying commercial Au foils, attaining unidirectional alignment and seamless stitching.107 Subsequently, Li et al. grew 2-inch MoS2 single crystals on c-plane sapphire with a miscut orientation towards the a-axis. By applying an ∼1° shear angle along this direction, they induced atomic steps that effectively broke the nucleation energy degeneracy. The resulting field-effect transistors exhibited excellent wafer-scale uniformity and a high mobility of 102.6 cm2 V−1 s−1, setting a record for monolayer CVD-grown MoS2.108 Inspired by this, Wang et al. proposed the concept of “Dual-Coupling Effect” to describe the complex synergy between epitaxial relationships and atomic steps and eventually enabled the preparation of large-size single crystal TMDC films, including WS2, MoS2, MoSe2, and NbSe2 (Fig. 3j).73 The epitaxial interaction between WS2 and vicinal a-plane sapphire surfaces gives rise to two preferred antiparallel orientations, while the sapphire step edges disrupt the symmetry of these orientations. These two interactions promote the unidirectional alignment of crystal islands, ultimately resulting in seamless fusion without grain boundaries.
Atomically thin 2D materials without interlayer dangling bonds are also ideal building blocks for constructing 2D/2D heterojunctions. Heterostructures can also be directly synthesized via bottom-up epitaxy by precisely controlling precursor supply, nucleation sites, and deposition sequence. Wafer-sized vertical heterostructures, such as MoS2/graphene, MoS2/WS2, WSe2/MoS2, and WSe2/MoSe2, have been successfully synthesized using chemical methods.115–119 Beyond vertical (out-of-plane) structures, TMDCs can also be used to construct atomic-scale lateral (in-plane) heterostructures. Unlike vertical structures, planar epitaxy requires a higher degree of crystal structure matching, where two different 2D single crystals form 1D linear bonding only at the interface (Fig. 3l). The growth of heterostructures as vertical (VHs) or lateral (LHs) depends on the growth kinetics and thermodynamics, with factors such as nucleation energy, diffusion, vdW interaction energies, and edge energy influencing the final structure's stability.74 For example, Gong et al. demonstrated a growth strategy for WS2/MoS2 heterostructures, achieving both out-of-plane heterostructures with strong excitonic transitions and in-plane heterostructures with localized photoluminescence enhancement by controlling the growth temperature.120 Li et al. successfully achieved precise control of the heteroepitaxy direction and effective manipulation of the diffusion barrier of active clusters by rationally controlling the metal/chalcogenide ratio in the vapor precursors.121
In summary, with the advancement of synthesis techniques, the family of 2D materials has been greatly expanded, with sizes extending from the micron scale in the laboratory to the wafer scale. Epitaxial growth methods have significantly improved the crystallinity, wafer-scale uniformity, optical and electrical properties, and expanded the range of complex 2D materials and heterostructures. However, due to the immaturity of low-temperature growth processes, the next major challenge hindering the commercialization of 2D materials is the high-yield, repeatable, residue-free, wrinkle-free wafer-scale 2D transfer technology.
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| Fig. 4 The philosophy of 2D transfer. (a) The successful pick up requires F2 > F1. (b) The successful release process requires F3 > F2. | ||
F1: the interaction between the 2D material and the original growth substrate, determined by chemical bonding or physical adsorption (e.g., vdW forces).
F2: the adhesion between the 2D material and the transfer medium (such as PDMS or polymer layers), regulated by polymer chemistry, surface energy, or electrochemical modulation.
F3: the adhesion between the 2D material and the target substrate, which can be enhanced through surface treatments (e.g., hydroxylation and amino-silanization) or chemical activity at defect sites.
For efficient pick-up, F2 should be larger than F1, allowing the intermediate medium to lift the 2D material from its original substrate. This can be achieved through methods like capillary force-assisted transfer, where water thin film provides the additional adhesion force to enhance the F2, or polymer-assisted transfer, where the interaction between the polymer and the 2D material is carefully designed to strengthen F2 by adjusting the temperature.122 Alternatively, reduce F1 through other methods until it becomes easy to overcome. For example, use liquid nitrogen to weaken the vdW force between the TMDCs and the growth substrate.123 If F1 is too strong to overcome, a common solution is PMMA-assisted wet transfer, where the growth substrate is chemically etched to effectively kill the F1 to zero.
During the release step, F2 should be smaller than F3, ensuring that the 2D material adheres preferentially to the target substrate. A common strategy is to reduce F2. For example, in the capillary-assisted method, the water vapor that initially serves as a temporary adhesive disappears after pick-up. As the vapor vanishes, the adhesive force drops significantly, resulting in a much lower F2.
Strategies such as solvation effects (intercalation of water molecules124,125), or thermodynamic disturbances (e.g., temperature-induced polymer chain movement126–129 and differences in thermal expansion coefficients130), are employed to weaken F2, allowing F3 to dominate and successfully complete the transfer. Furthermore, PDMS has strong adhesion when the peeling speed is fast and weak adhesion when the peeling speed is slow. By slowly releasing the 2D material, it is possible to effectively reduce F2, thus allowing the 2D material to remain on the target substrate.9
In some extreme cases, when the interaction force between the transfer medium and the 2D material is excessively strong and cannot be released without compromising the material quality, the transfer medium is typically removed or dissolved, thereby reducing the F2 value to zero. For instance, in the case of PMMA or metal transfer media, their inherently high F2 values necessitate removal by dissolution after the 2D material is brought into contact with the target substrate, rather than relying on the competition of interfacial forces.
By systematically controlling these interfacial forces, as schematically depicted in (Fig. 4), researchers can achieve high-fidelity, clean, and reproducible transfer of 2D materials to a wide variety of substrates, thus bridging the gap between material synthesis and device fabrication. In the following sections, we will elaborate on how this underlying philosophy is implemented across various state-of-the-art transfer methods, illustrating the practical strategies and innovations developed to address the unique challenges of 2D material integration (Fig. 5).
Building on this fundamental philosophy, several advanced transfer strategies have emerged in recent years, including the UV tape assisted wafer scale method,21 the Au assisted method,39 and the SiNx membrane assisted method,20 each offering unique advantages for specific applications.
To facilitate a systematic comparison, we present a comprehensive evaluation of each method using radar charts, assessing critical dimensions such as transfer cleanliness, ease of operation, achievable area, completeness, versatility across different types of 2D materials (e.g., CVD-grown vs. exfoliated), and potential for multifunctional integration.
However, the strong adhesion between graphene and copper introduces significant challenges during transfer.136 The most widely used solution is the wet transfer method, in which a polymer support layer, most commonly PMMA, is spin-coated onto the graphene/copper substrate. The copper is then chemically etched away, effectively reducing the interfacial force F1 (between the 2D material and the growth substrate) to zero and allowing easy delamination. Subsequently, the PMMA/graphene stack is floated onto deionized water and transferred to the target substrate. In the final step, dissolving the PMMA support layer in acetone eliminates the interfacial force F2 (between the 2D material and the transfer medium), ensuring that the graphene adheres preferentially to the target substrate, in accordance with the core transfer philosophy.
The PMMA-assisted wet transfer approach offers notable simplicity and versatility, making it a standard protocol for a wide range of 2D materials. It provides critical mechanical support, protecting fragile monolayers throughout the transfer process. However, this method is not without drawbacks. PMMA residues often persist even after extensive solvent rinsing, leading to contamination, p-type doping, and degraded electrical performance. Additional strain may also be introduced during curing and removal. These factors have spurred research into alternative polymers; examples include paraffin,137 polystyrene (PS),138,139 ploy(L-lactic acid) (PLLA) and L-lactide-ε-caprolactone copolymer (PLC),132 cellulose nitrate (NC),140 cellulose acetate butyrate (CAB),141 cellulose acetate (CA),142 and polyvinyl alcohol (PVA).143 However, they have corresponding disadvantages: paraffin wax can produce clean and large-area graphene, but due to its large expansion coefficient, temperature perturbations introduce greater stress and reduce the mechanical strength of graphene, so in order to improve mechanical strength, the integrity of the transferred 2D material is generally maintained by double-layer PMMA design.144,145 Polystyrene PS is usually brittle and difficult to apply in large-area transfer graphene applications, so it is necessary to increase its mechanical flexibility and add softener139 to the polymer to reduce cracks caused by the transfer process to graphene. NC introduces some strain-related characteristics because it is rigid as a polymer and cannot be relaxed by annealing. The overall surface wrinkles of CAB-transferred graphene are much less than those of PMMA transferred graphene, but the electrical properties are not much improved.
To further reduce contamination, polymer-free wet transfer techniques have emerged, using agents like rosin146 or cyclohexane.147 While these can lower surface residues, they tend to compromise mechanical strength or introduce other compatibility issues, such as the need for additional protective layers,148 or process constraints due to pH sensitivity.
In addition to polymer residues, chemical etching agents themselves can introduce unwanted contaminants during wet transfer. To address this, alternative methods have been explored. One promising approach is electrochemical bubble delamination, which generates gas bubbles at the interface between the 2D material and the substrate, physically lifting the film and thereby reducing the need for aggressive chemical etchants.11 This process can effectively weaken or even “kill” the interfacial force F1, facilitating delamination. However, it requires careful control, as the mechanical stresses generated by bubble formation can damage delicate 2D materials, necessitating continued reliance on a PMMA support layer for protection.149 Moreover, this technique is only compatible with conductive (metal) substrates, such as those used for graphene and h-BN, and is not suitable for insulating substrates like SiO2/Si, mica, or sapphire, which is commonly used for TMDCs. Additionally, any remaining etching steps can still damage the original metal substrate, limiting the method's repeatability and scalability. Improvements such as ultrasonic-assisted delamination have been developed to broaden substrate compatibility and accelerate the process,150 and some studies have focused on designing sacrificial layers or protective coatings to further minimize substrate damage.151
In summary, while wet transfer, particularly the widely used PMMA-assisted method, remains the most practical and scalable approach for transferring CVD-grown 2D materials, it continues to face persistent challenges. These include polymer contamination, strain induced during processing, and a lack of spatial precision, as the floating 2D films cannot be aligned accurately on the target substrate. Such limitations are especially problematic for applications demanding strict control over layer positioning, such as vdW heterostructure assembly or optoelectronic device fabrication. These ongoing challenges continue to drive innovation in both transfer protocols and post-transfer cleaning strategies.
Conventional wet-transfer techniques, which rely on retrieving floating 2D films from a liquid surface, suffer from significant limitations in spatial control and alignment. To overcome these challenges, deterministic dry transfer approaches have been developed. In these methods, 2D flakes are typically picked up by PDMS stamps and positioned with high precision, making them well-suited for constructing vdW heterostructures and other complex architectures.
The fundamental principle of mechanical exfoliation involves applying a force that exceeds the interlayer vdW attraction in the parent crystal, thereby producing atomically thin flakes while preserving in-plane crystallinity. Castellanos-Gomez et al.9 pioneered a dry transfer protocol using PDMS: bulk vdW crystals are mechanically exfoliated using adhesive tape, transferred onto a PDMS stamp, and then aligned and pressed onto the target substrate. The viscoelastic nature of PDMS facilitates both pick-up and release of the 2D material.
Despite its advantages in spatial precision, the PDMS-based approach faces key limitations. The intrinsic adhesion between PDMS and many 2D materials is relatively weak, which hinders its ability to reliably pick up flakes directly from growth substrates.152 To improve pick-up efficiency, one might increase PDMS stickiness, either by lowering the cross-linker ratio or optimizing the curing process, making it easier to exfoliate flakes.153 However, a more adhesive PDMS also tends to be “dirtier”: long-chain polymer fragments are more likely to transfer onto the 2D flake surface, leading to chemical contamination that degrades material and device performance.154 On the other hand, using a higher cross-linker content or higher curing temperature produces a cleaner PDMS surface but results in lower adhesion, making it more difficult to pick up 2D materials.155 This trade-off between cleanliness and adhesion presents a major challenge for PDMS-based transfer.
A practical solution to this dilemma is a two-step approach: first, exfoliate the 2D material onto a clean wafer using a “clean” (highly cross-linked, well-cured) PDMS, ensuring minimal contamination; then, transfer the desired flake from the wafer onto the target substrate using a more controllable and clean transfer medium. This strategy enables both high interface quality and reliable flake manipulation and has become increasingly popular for applications requiring both ultra-clean surfaces and spatial precision.
In this manner, a variety of alternative polymer supports have been explored. Polypropylene carbonate (PPC)126 offers tunable adhesion through temperature control, with adhesion remaining high at room temperature but dropping significantly when heated to ∼70 °C, which enables effective pick-up and easy release. PVA exhibits strong adhesion when melted at 90 °C and can be dissolved in water to yield a clean interface;14,156 however, it often requires additional support layers to ensure flatness and mechanical stability. Polycarbonate (PC) follows a similar principle but requires higher processing temperatures (∼150 °C), which may risk oxidation and degrade 2D material quality compared to the milder conditions used for PVA.127,157
In addition to polymer-assisted techniques, h-BN has gained prominence as both a pick-up and encapsulation material.158 Thanks to its atomically flat, chemically inert surface and robust van der Waals interaction with other 2D materials, h-BN is ideal for assembling clean and high-mobility devices.159,160 For instance, the mobility of graphene field-effect transistors can reach up to 140
000 cm2 V−1 s−1 when h-BN is used as the substrate and encapsulant, an order of magnitude higher than conventional SiO2-supported devices.160 The h-BN layer also offers a self-cleaning effect, mitigates charge traps, and provides protection against oxidation and environmental damage,160–165 The typical procedure involves first picking up h-BN with a PPC stamp, then using this h-BN “handle” to pick up the target 2D flake by van der Waals adhesion.
While h-BN-assisted dry transfer offers clear benefits in device performance and interface quality, it comes with its own limitations. The transfer area is constrained by the size of the h-BN flake, and after assembly, the h-BN is difficult to remove, making this approach unsuitable for applications where the 2D surface needs to be exposed, such as in chemical functionalization or catalysis.166 Additionally, the mechanical rigidity of h-BN imposes limitations on flexible device applications and large-area transfer.
In order to achieve large-scale dry transfer, Zhang et al. used selenium (Se) as the mediator and PPC as the support layer.167 They transferred the wafer-level single-layer MoS2 onto the target substrate using a water-soluble tape. Subsequently, they removed the PPC through reactive ion etching (RIE) and removed the selenium layer in a nitrogen atmosphere for annealing. This resulted in a highly clean MoS2 surface. Finally, through standard semiconductor processes, field-effect transistors (FETs) and logic circuits were fabricated on the transferred MoS2 film, achieving a switching current ratio of up to 2.7 × 1010 and an electron mobility of 71.3 cm2·V−1·s−1. The compatibility with existing semiconductor manufacturing processes was verified.
Overall, while dry transfer methods have revolutionized the deterministic assembly of 2D materials, enabling unprecedented control over spatial arrangement and interface quality, they are still evolving to address persistent challenges. These include improving the pick-up efficiency for large-area or substrate-bound films, minimizing polymer or PDMS contamination, and enabling more flexible, scalable, and reversible integration strategies. Continued innovation in transfer media, temperature control, and van der Waals engineering is expected to further expand the capabilities and application scope of dry transfer technologies for 2D materials.
Recognizing the complementary strengths and limitations of these two paradigms, hybrid capillary-force-assisted transfer methods have emerged as a powerful solution, leveraging the best of both approaches. The essence of these techniques is to temporarily use a thin film of evaporative liquid, such as water, acetone, or isopropanol vapor, as an “instant glue” between the PDMS stamp and the 2D material during the pick-up process. The capillary force dramatically increases the effective adhesion (F2) during pick-up, easily exceeding the interfacial force with the growth substrate (F1), thereby enabling efficient exfoliation even for challenging geometries or hollow substrates. After the liquid evaporates, the adhesion force drops, greatly reducing (F2), which allows the 2D material to be cleanly released onto the target substrate (where F3 > F2), thus providing a dynamically tunable transfer force throughout the process.
A landmark study by Ma et al. introduced this concept by condensing a thin layer of water vapor onto a clean PDMS stamp.124 The water layer provides strong, but transient, capillary adhesion for picking up graphene or TMDCs from SiO2/Si substrates, previously impossible with standard dry PDMS. Once the water evaporates, the 2D flake can be precisely and gently placed on the target substrate. Critically, because only volatile liquids are used, this process eliminates polymer contamination and avoids post-transfer annealing, preserving the pristine surface and high mobility of the 2D material. Devices fabricated using this approach have demonstrated record-high carrier mobility and minimal charge neutrality point shift, confirming ultra-clean interfaces. Furthermore, by patterning the PDMS stamp into arrays, selective pick-up and deterministic assembly of device arrays or lithography-free fabrication becomes possible.
Building upon this foundation, a recent work further advanced the field by employing a patterned PDMS stamp (micro-post arrays) and introducing a capillary-force-assisted mass transfer printing (MTP) technology.133 In this approach, an ethanol–water solution is introduced at the interface, which penetrates non-contact regions between the PDMS micro-posts and the 2D film, causing controlled delamination by capillary action. This enables wafer-scale transfer and patterning of monolayer MoS2 and vdW heterostructures, with transfer yields approaching 99% and negligible device degradation, even for over a million device arrays in a single step. By tuning the type and ratio of the volatile liquids (e.g., water, ethanol, and isopropanol), the method can be adapted to 2D materials sensitive to water (such as black phosphorus) and can even be performed in inert atmospheres inside gloveboxes. The use of ultraclean, patterned PDMS further reduces contamination and enables selective, scalable device integration.
A notable advantage of the capillary-force-assisted hybrid approach lies in its use of exceptionally clean, highly crosslinked PDMS stamps, which significantly reduces polymer contamination compared to conventional sticky PDMS-based methods. This is particularly important for preserving the intrinsic electronic properties of high-mobility 2D devices. Furthermore, the capillary medium is highly adaptable: while water vapor often serves as the “instant glue” to provide temporary adhesion, the process can easily be carried out with other volatile solvents such as isopropanol (IPA) or acetone vapor, especially in an inert glovebox environment. This versatility enables the transfer of water-sensitive materials, such as black phosphorus, using compatible vapors that prevent degradation. The combined use of ultra-clean PDMS and tunable capillary media ensures a gentle, contamination-free, and highly efficient transfer process across a broad range of 2D materials and device integration scenarios.
In summary, capillary-force-assisted hybrid methods represent a near-ideal solution for 2D material transfer: they offer tunable interfacial forces for efficient pick-up and release, minimize contamination, and are compatible with both large-area and patterned integration, as well as sensitive or air-unstable materials. This new class of techniques address nearly all key challenges of previous wet and dry transfer methods, opening the door to high-throughput, contamination-free, and lithography-free fabrication of advanced 2D material devices.
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| Fig. 6 Recent advanced transfer methods. (a) The dielectric-assisted transfer method. (I and II) The schematic illustration of the lattice symmetry and epitaxial growth of Sb2O3 on Cu(111) (I) and graphene-covered Cu(111) (II). (III) The photo of the 4-inch as-deposited s-Sb2O3 on graphene-covered Cu(111) wafer. (IV) The z-contrast atomic-level HAADF-STEM image of Sb2O3 showing the atomically resolved lattice. (V) The schematic illustration of the atomic structure of Sb2O3 grown on graphene-covered Cu(111). (VI) The representative image of the transferred graphene. Reproduced from ref. 168 with permission from Springer Nature, Copyright 2025. (b) The SiNx membrane-assisted transfer method. Scanning electron microscope (SEM) (I) and optical (II) micrographs of the cantilevers after picking up thick (∼40 nm) h-BN crystals. (III) The optical micrograph showing the cantilever in contact with graphene (edges highlighted with a dashed line) on SiO2. The flexible nature of the cantilevers allows accurate control of the lamination process. (IV) The optical micrograph showing the resulting heterostructure on an oxidized silicon wafer with large uniform areas. Adapted from ref. 20 according to Creative Commons Attribution 4.0 International License (CC BY 4.0). (c) The UV tape-assisted transfer method. (I) Three graphene/Cu(111) substrates with UV tapes, used for large-area three-layer stacked graphene. (II) The photo of the graphene stack made by transferring three sheets of large monolayer graphene. (III and IV) The transferred single-crystal monolayer graphene grains. (III and IV) The optical and atomic force microscopy (AFM) imaging. Adapted from ref. 21 according to Creative Commons Attribution 4.0 International License (CC BY 4.0). | ||
000 cm2 V−1 s−1 and MoS2 FETs with steep subthreshold swings and high on/off ratios. Such dielectric-mediated strategies offer a scalable and contamination-free platform for next-generation 2D electronics.
In summary, these advanced transfer methods share several key advantages: high material versatility, streamlined operation, large-area and high-quality transfer capability, and minimal interfacial contamination or damage. As shown in Fig. 6, the latest techniques now enable scalable, precise, and contamination-free transfer of 2D materials for state-of-the-art device integration and commercial applications.
No single transfer method is universally superior in all categories. Instead, each method presents a distinct set of trade-offs tailored for specific research or industrial needs. For applications prioritizing cleanliness and high electronic performance, h-BN pick-up and dielectric-assisted methods are preferred. For large-area and scalable integration, capillary force-assisted and UV tape strategies offer major advantages. When process simplicity and versatility are essential, wet transfer remains widely used, despite its drawbacks in interface quality. In addition, we have summarized in the supporting information (Table S2) representative studies of 2D material FETs, compiling device-level metrics such as carrier mobility, contact resistance, threshold voltage shift, noise levels, and long-term cycling stability, to provide readers with direct correlations between transfer strategies and device performance.
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| Fig. 8 Transfer beyond 2D materials. (a) The photonic crystals (PhCs). Suspended PhCs are detached from GaP and transferred onto SiO2/Si substrates, enabling integration with light-emitting vdW heterostructures and cavities. Reproduced from ref. 170 with permission from American Chemical Society, Copyright 2017. (b) Nanowire mesh. A large-area nanowire mesh device is fabricated and transferred, as shown in top-view and cross-sectional SEM images. Reproduced from ref. 178 with permission from American Chemical Society, Copyright 2017. (c) Si flakes. An ultrathin Si flake is transferred onto PtSe2 to form a UV photodetector. Reproduced from ref. 172 with permission from Wiley-VCH, Copyright 2024. (d) Diamond film. An ∼1 µm-thick, 2-inch-wide diamond membrane is exfoliated from Si using adhesive tape, leaving the substrate clean and reusable. Reproduced from ref. 171 with permission from Springer Nature, Copyright 2017. | ||
A landmark example is the transfer of photonic crystal cavities, treated as van der Waals flakes, as demonstrated by Liu et al.170 Using classical PDMS dry transfer, vertically stacked heterostructures were first assembled on an Si/SiO2 substrate, after which prefabricated photonic crystals were picked up and precisely transferred onto the 2D stack. This enabled localized enhancement of electroluminescence in the nanocavity, illustrating the power of transfer for multifunctional device integration (Fig. 8a). In addition, transfer techniques have further expanded to one-dimensional and multilayer photonic devices. Yang et al. applied an improved transfer printing method for integrating 1D photonic crystal films onto organic translucent photovoltaic devices, using PDMS as a support for roll-to-roll (R2R) compatible, low-temperature transfer.173 Similar strategies have been extended to membrane reflectors, multi-layer laser cavities, and even wafer-scale transfer of compound semiconductor layers.175,176 For advanced nanomaterials, such as MXenes, wet transfer protocols have enabled large-area, flexible, and conductive films. Xu et al. prepared Ti3C2Tx MXenes on glass, then employed PMMA-assisted wet transfer onto diverse targets.177 In optoelectronics, dry transfer has been used to fabricate transparent conductive electrodes (TCEs) based on Ag nanowires, offering excellent electrical and mechanical properties (Fig. 8b).178 Even traditional semiconductor wafers have benefited: Wang et al. used a combination of wet etching and dry PDMS transfer to assemble ultra-thin silicon wafers onto patterned PtSe2, followed by further device integration steps to realize high-speed UV photodetectors (Fig. 8c).172 Notably, transfer methods have even enabled the manipulation of robust materials such as diamond. Jing et al. devised a single-edge burst stripping technique, using tape to peel off wafer-scale diamond films, which can then be integrated onto various substrates (Fig. 8d).171 This process produces ultra-flexible, large-area diamond films compatible with strain engineering and flexible sensing.
Overall, these examples underscore the remarkable generality and transformative potential of transfer techniques. By refining steps originally developed for 2D materials, researchers are now able to integrate a diverse array of functional films and nanostructures, ranging from atomically thin layers to macroscale membranes, opening new frontiers in electronics, optoelectronics, and flexible devices by transferring for almost “everything”.
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| Fig. 9 Transfer materials on arbitrary devices. (a) Transfer to ring resonators. Schematic and device design showing a WS2 monolayer integrated with a SiNx ring resonator for ionic-liquid-controlled modulation. Reproduced from ref. 181 with permission from Springer Nature, Copyright 2020. (b) Transfer materials to waveguides. Scheme and experimental demonstration examples of transferred WSe2 or graphene flakes on waveguides. Adapted from ref. 182 according to Creative Commons Attribution 4.0 International License (CC BY 4.0). Reproduced from ref. 185 with permission from Springer Nature, Copyright 2011. (c) Transfer material on suspended devices. Schematic and device design of transferring the 2D twisted device or monolayer on holes or a hole array (PhC cavity). Reproduced from ref. 180 with permission from Springer Nature, Copyright 2015. Reproduced from ref. 186 with permission form Springer Nature, Copyright 2022. | ||
One significant challenge in integrating 2D materials onto functional devices is the inherent non-planarity and structural complexity of many target surfaces. Device architectures such as photonic crystals with pillar or hole arrays, or waveguides with pronounced topography, often present a low fill factor or rough, uneven profiles.183 As a result, the average interfacial adhesion force (F3) between the 2D material and the device surface is substantially reduced, making reliable and residue-free transfer particularly difficult. In such cases, conventional transfer methods may fail to achieve uniform contact or clean release. To address this, it becomes essential to adopt transfer strategies that can further minimize the adhesion between the 2D material and the transfer medium (F2)—for example, through hybrid or capillary force-assisted techniques, substrate heating, or the use of sacrificial layers—thereby ensuring successful transfer even onto substrates with minimal or discontinuous contact area.132,184 The versatility of 2D materials, stemming from their atomic thickness and vdW interactions, allows them to conform to a variety of substrates, but optimal integration requires careful engineering of interfacial forces tailored to the specific device geometry.
Here, we highlight some representative examples for transfer onto arbitrary substrates, including ring resonators, waveguides and suspend devices. Electro-optic modulation and ring resonators: Datta et al. integrated monolayer WS2 onto a silicon nitride microring resonator using polymer-assisted wet transfer, demonstrating strong light–matter interaction between 2D materials and ring resonators and the electrical tunable opto-device (Fig. 9a).181 Graphene-based modulators, first demonstrated by Liu et al., were realized by transferring monolayer graphene onto optical fiber waveguides, enabling the development of the first integrated graphene electro-absorption modulator.185 Besides, single-photon emitters on waveguides: Peyskens et al. used dry transfer to place WSe2 onto silicon nitride photonic integrated circuits, realizing deterministic integration of single-photon emitters (Fig. 9b).182 Sun et al. employed mechanical exfoliation and dry transfer to place WS2/WSe2 heterojunctions onto circular hole arrays, observing interlayer exciton enhancement in suspended geometries (Fig. 9c).186 Similarly, dark exciton readout and quantum photonics: Ma et al. transferred exfoliated WSe2 and h-BN films onto silicon nitride PhC using capillary force-assisted clean stamp transfer.179 This enabled the realization of a dark exciton qubit readout system. Nanolaser has also been achieved by Wu et al. through the traditional polymer wet transfer. They integrated WSe2 onto prefabricated photonic crystal cavities, serving as a gain medium for nanolasing after polymer removal.180
Addressing these industrial requirements has motivated the exploration of next-generation transfer strategies that combine cleanliness, scalability, and broad material compatibility. Very recently, the team led by Zheng et al. proposed a transfer method based on the electrostatic double layer (EDL) repulsion mechanism (EDL transfer), which utilizes the EDL repulsive force formed in ammonia solution to achieve non-destructive separation of vdW materials from the growth substrate.195 Importantly, this method does not rely on etching reactions. The EDL repulsive force is based on making both the material and the substrate surface negatively charged to form a long-range electrostatic repulsion force, overcoming van der Waals attraction, thereby achieving material exfoliation, avoiding the problems of etching damage, contamination and residue in traditional methods. It not only improves the integrity and interface cleanliness of the material but is also applicable to various 2D materials (TMDs, graphene, h-BN, CNT, etc.) and substrates (oxides, metals, nitrides, mica, etc.). By adjusting the pH and ionic strength of the solution, the EDL repulsive force can be effectively enhanced to achieve rapid, uniform, wafer-level material exfoliation. Moreover, the entire process is rapid and mild and can achieve centimetre-level exfoliation in just a few seconds.
The advent of automation and AI-enabled process control further amplifies this transformation.201 By enabling precise, reproducible handling of delicate 2D layers, minimizing human error, and allowing real-time process optimization, automated transfer systems not only boost yield and uniformity, but also facilitate the complex multi-step stacking and assembly required for next-generation electronic and optoelectronic devices. These advances are directly aligned with the evolving requirements of the global semiconductor industry, as reflected in the IRDS.90,91
In this section, we will highlight how large-scale transfer approaches, especially R2R and AI-driven automated transfer, are poised to unlock the industrial potential of 2D materials, ensuring their successful integration into the semiconductor roadmap and setting the stage for the next wave of electronic and quantum technologies.
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| Fig. 10 Large-scale preparation (a). The concept of the roll-to-roll (R2R) transfer. (b) The concept and design of AI-driven automated transfer systems. Reproduced from ref. 201 with permission from Springer Nature, Copyright 2025. | ||
Early breakthroughs in this field were exemplified by Bae et al. who achieved the transfer of 30-inch graphene films using a wet-etching process to remove the copper growth substrate, followed by direct lamination onto polymer films.200 Subsequent advancements by Kobayashi and colleagues introduced photocured epoxy resin adhesives, which substantially improved transfer yield and enabled the production of graphene films up to 100 meters in length, marking a significant step towards true industrial-scale production.202 For TMDs like MoS2, whose vapor-phase growth chemistry complicates direct R2R integration, hybrid wet/dry R2R strategies have been devised, allowing for the continuous transfer of large-area MoS2 layers with high crystallinity and device-grade performance.
Despite these substantial advances, the R2R paradigm presents technical challenges, particularly those inherited from wet-transfer processes, namely, polymer residue contamination, difficulties in maintaining interface cleanliness, and the single-use nature of etched metal substrates. These issues can degrade the electrical and mechanical properties of the transferred 2D layers, limiting their utility in high-performance devices. Recent innovations, such as dry R2R methods that enable precise control of peel tension and speed, are mitigating these limitations and yielding higher-quality films. Additionally, techniques like electrochemical delamination and etchant-free hot water separation have enabled the reuse of metal growth substrates and reduced the risk of ionic contamination, further enhancing process sustainability and scalability.
Nevertheless, R2R transfer remains largely confined to 2D materials and substrate combinations compatible with continuous roll architectures. Translating these advances to rigid wafers or arbitrary substrates presents ongoing challenges, particularly in terms of alignment, uniformity, and defect minimization over meter-scale areas. Achieving pristine interfaces free from mechanical defects such as wrinkles, tears, and bubbles remains a critical area of technical development for the next phase of industrial integration.
Liu Zhongfan's team recently reported a fully automated transfer platform that addresses these bottlenecks by integrating advanced robotics, programmable feedback control, and precision engineering of interfacial forces201 (Fig. 10b). Their approach introduces a tunable Al/Al2O3 adhesion layer, enabling programmable internal strain and precise delamination/lamination control. Combined with robotics for handling, spin-coating, lamination, and peeling, the system achieves crack-free, residue-free, and highly uniform wafer-scale transfer of CVD-grown graphene, h-BN, MoS2, and their vdW heterostructures.
Notably, the system demonstrates a production capacity of up to 180 wafers per day, with >99% intactness and carrier mobilities for transferred graphene exceeding 14
000 cm2 V−1 s−1 across a 4-inch wafer, with performance metrics comparable to or even surpassing those of manually exfoliated materials. The automated, solution-free process eliminates harsh chemical etchants and minimizes environmental impact, as verified by comprehensive life cycle assessment (LCA).
AI- and robotics-assisted transfer systems set new benchmarks for precision and repeatability in 2D materials integration, as these platforms tightly regulate tension, speed, and pressure during each transfer step, dramatically reducing defects such as cracks, bubbles, and wrinkles that often plague manual approaches and ensuring high device reliability at scale.201 The resulting material and substrate flexibility is notable: automated workflows can seamlessly handle graphene, h-BN, MoS2, and complex heterostructures, with compatibility across a broad spectrum of substrates, including Si, SiO2/Si, HfO2, and Al2O3. Layer-by-layer stacking and heterostructure assembly become both programmable and highly reproducible. From an industrial viability standpoint, these automated solutions achieve high throughput, robust wafer-to-wafer consistency, and ultra-low contamination, effectively bridging the gap between academic demonstrations and practical manufacturing for photonics, electronics, and quantum technologies.203 Importantly, sustainability is enhanced by minimizing liquid-phase waste and reducing labour costs, yielding a more environmentally friendly and economically attractive process than traditional chemical-based transfers. Nevertheless, challenges remain, including adapting these platforms to rigid, non-rollable substrates, automating multi-material assembly, and developing closed-loop, AI-driven defect detection to ensure quality and scalability for future industrial applications.
In summary, the emergence of automated, AI-assisted transfer and analysis platforms represents a paradigm shift in the scalable production of 2D materials.204,205 These systems will be foundational to integrating 2D materials into the semiconductor roadmap and unlocking their full commercial potential in next-generation flexible, transparent, and quantum electronic devices.
Specifically, water and hydrocarbons in the air can quickly contaminate the surface of 2D materials, causing the hydrophilic surface of 2D materials to become hydrophobic.207,208 By controlling the relative humidity of the environment at a lower humidity level, the density of tiny water droplets in the air can be reduced, and materials with hydrophilicity will not adsorb the moisture in the air.209 In our laboratory experience, environmental humidity has a profound influence on the stability of exfoliated 2D flakes. For instance, in Singapore, where the relative humidity often exceeds 50–60%, freshly exfoliated flakes exhibit markedly shorter lifetimes compared to those prepared under the much drier conditions in Canberra, Australia (lab humidity is ∼30%). The higher ambient moisture promotes surface adsorption and interfacial oxidation, accelerating degradation and leading to faster loss of optical and electronic integrity. This observation highlights the critical role of environmental control in preserving the intrinsic properties of 2D materials during storage and device fabrication.
In addition to humidity, the oxidation is another obvious factor that can downgrade the 2D flack qualities.210 When oxygen undergoes chemical adsorption with the material, an irreversible oxidation reaction occurs, forming localized states at the surface or defects, becoming electron/hole scattering centers or traps, reducing the mobility and causing threshold drift, ultimately leading to a decline in the performance of the device.211–216 For example, when graphene is oxidized or PMMA is left with carbon, non-radiative recombination increases, photoluminescence (PL) is quenched, the spectral line broadens or an additional background appears.214
Moreover, the oxidation of 2D materials is strongly accelerated under certain environmental conditions. Elevated temperatures can enhance oxygen diffusion and reaction kinetics, leading to rapid degradation of materials such as MoS2 and black phosphorus (BP) through the formation of oxides or suboxides.217–219 High humidity further exacerbates oxidation, water facilitates oxygen-water redox chemistry and aids defect-assisted hydrolysis/oxidation pathways, producing hydroxylated species that speed up layer etching and chemical degradation, a particularly severe problem for hydrophilic materials such as BP.219 Therefore, controlling ambient temperature, oxygen partial pressure and relative humidity during transfer and post-processing, together with timely encapsulation, is essential to limit irreversible oxidation and to preserve intrinsic electronic and optical properties.
The significance of such encapsulation was first demonstrated by Dean et al., who found that the direct contact between graphene and the substrate introduced significant impurity scattering and reduced carrier mobility.160 By inserting h-BN as both a substrate and a capping layer, they obtained graphene devices with substantially improved performance, reflected in narrower charge neutrality peaks and higher induced charge densities under magnetic fields. This work laid the foundation for van der Waals heterostructure research and firmly established h-BN encapsulation as a gold standard in 2D material device fabrication.
However, while h-BN encapsulation greatly improves stability, its effectiveness is often compromised in practical device configurations (Fig. 11a). When the encapsulation layer is laminated over topographically uneven regions, particularly over thick metal electrodes, differences in rigidity, adhesion, and surface energy create local voids and interfacial gaps. These nanoscale pockets allow oxygen and water molecules to infiltrate, weakening the encapsulation and leading to localized doping, oxidation, or delamination over time. Such microcavities not only degrade contact reliability but also introduce trapped charge regions that deteriorate long-term device stability.221
To address these challenges, three complementary strategies have been developed (Fig. 11b–d): thinning the electrodes, forming 1D edge contacts, and introducing in situ via contacts.
Thinner electrode strategy (Fig. 11b): the most straightforward approach is to reduce the electrode thickness to minimize the step height at the metal/h-BN interface.222 Conventional electrodes, often tens of nanometers thick, can be replaced by ultrathin gold layers a few nanometers in thickness, or even by atomically thin conductive films such as few-layer graphene or emerging 2D metals like Au or Ga.223–225 These atomically flat electrodes ensure conformal contact between the top encapsulation and the active 2D channel, suppressing the formation of voids and interfacial strain. Recently, Zhao et al. developed a vdW compression technique capable of compressing metals such as Bi, Ga, In, Sn, and Pb to the atomic-thin limit (∼1 Å) between MoS2 anvil layers,226 offering a new pathway for creating perfectly matched ultrathin contacts compatible with encapsulation processes.
In addition, graphene can also serve as an encapsulation material. Mirzayev demonstrated a suspended 0D/2D heterostructure in which graphene layers were encapsulated and used to replace metal electrodes.227 This structure integrated C60 molecules between the two layers of graphene in a buckyball sandwich structure. The graphene layers protected the C60 molecules from damage caused by microscope vacuum and radiation, allowing for a direct study using STEM and imaging at the atomic resolution. Gyeon et al. used PtSe2 films as electrodes/contacts to fabricate FET devices and prepared a FET array with PtSe2 channels.228 The on/off ratio under p-type behavior reached approximately 103. This demonstrates that the electrode material can not only be used for semiconducting properties but also as an electrode or contact metal in certain devices.
Edge contact strategy (Fig. 11c): an alternative route to preserve interfacial integrity is to contact the 2D channel along its exposed edge rather than the top surface. Wang et al. first demonstrated this one-dimensional edge contact configuration, in which graphene encapsulated within h-BN was etched to expose its edges before metallization.169 This geometry eliminates the need for metal deposition on top surfaces, achieving both full encapsulation and excellent electrical coupling. The resulting devices exhibited record-high room-temperature mobilities of up to 140
000 cm2 V−1 s−1, attributed to the reduced contact-induced disorder and absence of trapped interfacial residues.
In situ via contact strategy (Fig. 11d): building upon the edge-contact concept, Telford et al. proposed integrating pre-patterned metal vias within the h-BN encapsulation layer itself, forming direct vertical contacts to the 2D channel beneath.229 This approach avoids local delamination caused by electrode topography, enabling intimate coupling with minimal contamination. Li et al. later advanced this technique using in situ through-hole metallization to embed contacts within h-BN, achieving excellent reproducibility, mechanical robustness, and long-term reliability.230 Such in situ via architectures are particularly promising for scalable, wafer-level integration, offering compatibility with industrial semiconductor processing.
In addition to the h-BN based encapsulation, graphene or even the functional devices themselves can serve as the protection layers. Recently, Bai et al. utilized a photonic crystal defect cavity (1D PhC defect cavity) to enhance and stabilize the second harmonic generation (SHG) performance of NbOCl2.220 By placing a thin NbOCl2 sheet between the upper and lower TiO2/SiO2 stacked mirrors to form a vertical resonant cavity, the incident light strongly resonates within the NbOCl2 layer, resulting in a 12-fold SHG enhancement. Moreover, the outer photonic crystal cavity served as a physical encapsulation layer, ensuring that the SHG signal of NbOCl2 did not show significant attenuation for 10 months in a room-temperature air environment.
In summary, although encapsulation remains essential for preserving the intrinsic properties of 2D materials, achieving defect-free sealing across realistic device geometries requires precise engineering of contact topology and interfacial conformity. Strategies such as ultrathin or 2D-metal electrodes, 1D edge contacts, and in situ via embedding have collectively pushed encapsulation performance to new limits. Altogether, these advances form the technological basis for achieving air-stable, durable, and high-mobility 2D electronic and optoelectronic systems.
Etching-based wet transfer introduces additional concerns.233 Metal ions (K+ and Na+) from common etchants can unintentionally dope 2D semiconductors and are incompatible with CMOS processes. In large-area MoS2 transfers, such residues increase surface roughness and contact resistance while degrading carrier mobility. Liu et al. recently demonstrated that incomplete rinsing steps can leave residual PMMA islands on graphene, creating localized charge traps and potential fluctuations that alter both Raman and PL signatures.234 These findings underline that polymer residues and interfacial impurities remain one of the most persistent obstacles in 2D material transfer.
During the transfer process, particularly in wet transfer, surface tension and capillary forces inevitably introduce local stress within the 2D material, leading to the formation of wrinkles, cracks, and interfacial bubbles. Such structural distortions significantly influence electrical and optical performance. Wrinkles and cracks increase resistance and carrier scattering, resulting in anisotropic conductivity and reduced carrier mobility.237,238 The strain accumulated along folds can also bend the local band structure of TMDCs, generating “quasi-quantum-dot” emission hotspots that alter the local PL energy and brightness, and in some cases, cause reconfiguration of the energy levels at the deformed regions.239,240 Internal crystal defects, including twin boundaries and irregular grain boundaries, further disturb Raman responses and disrupt lattice symmetry.241 Interfacial bubbles, on the other hand, enlarge the physical separation between adjacent layers, degrading optical coupling and introducing non-radiative recombination centers. These trapped voids increase PL and absorption interface states, diminish overall membrane response,242 and deteriorate charge transport by lowering field-effect mobility.243
Optical microscopy, along with a range of non-contact spectroscopic techniques, provides the most rapid and convenient means of assessing the quality of transferred films.238 Raman spectroscopy and photoluminescence (PL) mapping are particularly effective for detecting contamination and local strain or doping. For instance, variations in the D, G, and 2D bands of graphene, or shifts in excitonic peak positions in TMDCs, can indicate the presence of carbonaceous residues, strain accumulation, or charge-transfer doping.245 While these optical probes can distinguish between physical adsorption and charge doping, they are less effective at identifying the chemical composition of contaminants.246,247
X-ray photoelectron spectroscopy (XPS) complements optical methods by providing information on elemental composition and bonding states. Characteristic peaks such as C 1s, O 1s, C–O, and C
O reveal organic residues (e.g., PMMA fragments) or oxidation products.247 However, XPS suffers from limited spatial resolution and must often be combined with local probes. Photothermal-induced resonance (PTIR) offers a nanoscale alternative, capable of mapping the infrared spectra of surface pollutants with nanometer-scale resolution and high mass accuracy.248
Morphological methods such as atomic force microscopy (AFM) and scanning electron microscope (SEM) remain indispensable for identifying nanoscale residues, wrinkles, or bubbles through surface roughness mapping.249 Advanced photoelectron and work-function imaging techniques, such as X-ray photoemission electron microscopy (XPEEM), further enable correlation between surface chemistry and electronic structure.247 Cathodoluminescence (CL), when combined with SEM or scanning transmission electron microscopy (STEM), allows high-resolution optical characterization of encapsulated TMDs and h-BN heterostructures.250
Finally, secondary ion mass spectrometry (SIMS) provides high spatial and depth resolution, coupled with broad chemical sensitivity across elements, isotopes, and molecules, serving as a powerful complement to the above approaches.251
In summary, these characterization tools form a comprehensive framework for diagnosing contamination in transferred 2D materials, bridging structural, chemical, and electronic perspectives to guide cleaner and more reliable transfer protocols.
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| Fig. 12 Post-processing for clean strategies. (a) The thermal annealing method: thermal annealing gradually reduces surface roughness and removes residues at elevated temperatures. Reproduced from ref. 252 with permission from American Chemical Society, Copyright 2011. (b) The electrostatic force-assisted method: electrostatic force cleaning enables PMMA removal and yields cleaner graphene compared to solvent treatment. Reproduced from ref. 255 with permission from Wiley-VCH, Copyright 2013. (c) The plasma treatment method: plasma treatment produces large-area clean graphene films with preserved monolayer integrity. Reproduced from ref. 256 with permission from Elsevier, Copyright 2012. (d) The electrochemical treatment method: electrochemical treatment eliminates residues through electrolytic cleaning, lowering surface roughness. Reproduced from ref. 257 with permission from IOP Publishing, Copyright 2017. (e) The AFM-based mechanical treatment: AFM sweep (“nano-broom”) mechanically removes fabrication residues, improving device characteristics. Reproduced from ref. 258 with permission from IOP Publishing, Copyright 2011. | ||
The electrostatic-assisted cleaning approach (Fig. 12b), achieved by placing a statically charged cloth above the contaminated region, enables non-destructive PMMA removal at room temperature through electrostatic attraction. Plasma treatments (Fig. 12c), employing oxygen, hydrogen, or mixed gas chemistries (e.g., H2–N2 and H2–Cl2), offer highly effective removal of persistent organic and silicon-derived contaminants that survive conventional solvent cleaning or annealing. However, prolonged exposure can etch or unintentionally dope the 2D lattice. AFM/nanoprobe-based mechanical cleaning (Fig. 12e) allows localized and direct debris removal using atomic force microscope tips, particularly flexible or nanowire-coated probes, without substantial chemical modification. The combined “nano-ironing” approach, integrating thermal annealing with tip-assisted cleaning, further enhances surface planarity while minimizing oxidation and scratching. Although these methods of cleaning two-dimensional materials through mechanical force are more effective, they share a common drawback: the cleaning area is small, making them difficult to apply to large-scale cleaning of 2D materials.
Electrochemical cleaning (Fig. 12d) employs a voltage-driven water decomposition process to generate hydrogen bubbles that physically lift polymer residues off the surface. Although this technique is effective, precise control of the applied potential is necessary to prevent local delamination or structural damage.
Despite their maturity, chemical cleaning methods still face limitations such as incomplete residue removal, potential secondary contamination, and possible chemical damage to sensitive 2D lattices. These challenges have driven the search for more efficient and non-destructive alternatives. Recently, Fu et al. demonstrated an ultraviolet-based method to repair degraded sapphire substrates.254 Air exposure leads to hydrolysis of sapphire, disrupting epitaxial alignment and degrading its use as a growth template. However, by irradiating the substrate with 320–400 nm UV light for 30 minutes followed by heat treatment, its crystalline order can be fully restored. Using this repaired sapphire, 2-inch wafer-scale WS2 films were grown with exceptional uniformity and crystallinity, achieving >95% device yield and mobility fluctuations below 20%.
In summary, despite significant progress, no post-treatment can guarantee complete removal of PMMA or other organic residues. High-temperature or plasma treatments may only partially eliminate pollutants and can introduce new structural defects or chemical doping. Mechanical and electrochemical approaches offer promising alternatives but still carry risks of physical or chemical damage to delicate 2D structures.
Therefore, while post-processing greatly improves cleanliness and device performance, it often adds complexity and new sources of variability. The persistent challenge of achieving truly residue-free and undamaged interfaces underscores the urgent need for the development of fundamentally contamination-free, clean transfer methods as the field moves forward.
We must therefore acknowledge that post-transfer treatments can only partially restore interfacial quality and cannot fully reverse contamination or stress accumulation. Rather than relying on repair after transfer, the focus should shift toward preventing contamination at its source. This calls for the development of fundamentally clean, residue-free transfer methodologies using self-depolymerizing or volatile media, functionalized 2D support membranes, and automated, AI-driven platforms that minimize human variability. In parallel, in situ monitoring systems, based on Raman spectroscopy, optical interferometry, or electron microscopy, should provide real-time feedback to ensure closed-loop optimization. Collectively, these advances will enable reproducible, contamination-free integration of 2D materials at the wafer scale, bridging laboratory precision with industrial manufacturability.
The deliberate manipulation of 2D material morphology and stacking, whether by inducing controlled wrinkles, bubbles, strain fields, or twist angles, has emerged as a powerful toolkit for tailoring electronic, optical, and vibrational properties. Twist stacking, in particular, introduces a novel degree of freedom for tuning interlayer interactions and band structure in 2D materials.259 By precisely controlling the relative rotational angle between stacked layers, researchers can engineer moiré superlattices that give rise to emergent phenomena such as correlated insulating states, unconventional superconductivity, and tunable optical responses.260–262 Unlike traditional bulk materials, the atomically thin nature of 2D systems allows for deterministic fabrication and fine-tuning of these twist angles, unlocking rich new physics and functionalities for both fundamental research and device innovation.
In this section, we review the strategies and multifunctional applications enabled by transfer-induced engineering, focusing on wrinkles and bubbles, bending and folding, strain, and twist stacking. We summarize recent advances in the controlled creation, characterization, and utilization of these structural features, highlighting their impact on the physical properties and device performance of 2D materials.
The formation and control of wrinkles during transfer have been systematically studied. Wang et al. investigated wrinkle evolution in wedge transfer using a CAB polymer support.263 By floating the polymer/graphene stack on water and gradually lowering the water level, pre-existing wrinkles act as drainage channels, guiding the outflow of water and thus influencing the final wrinkle orientation and density (Fig. 13a). Notably, the hydrophilicity or hydrophobicity of the substrate strongly affects wrinkle formation—hydrophobic substrates suppress wrinkles, whereas hydrophilic substrates promote them.
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| Fig. 13 Transfer 2D material for wrinkle and bubble engineering. (a) The liquid phase wrinkle approach. The formation of graphene wrinkles is controlled by the wedge transfer method. Reproduced from ref. 263 with permission from AIP Publishing, Copyright 2012. (b) The mechanical wrinkle approach: the schematic and experimental demonstration of the mechanical method to achieve wrinkles on 2D flakes. The enhanced second-harmonic generation (SHG) signal has been achieved in NbOI2 flakes with wrinkle-induced strain. Reproduced from ref. 269 with permission from Springer Nature, Copyright 2022. (c) The bubble engineering: bubbles improve the mobility of r-MoS2. Reproduced from ref. 276 with permission from Springer Nature, Copyright 2022. | ||
Wrinkle engineering is not limited to graphene. Other 2D materials, such as transition metal oxides and dichalcogenides, also form wrinkles under stress.268 For example, buckling-induced delamination can introduce strong uniaxial strain in NbOI2, with the folded region reaching 3.1% strain and showing a 35-fold increase in SHG efficiency (the absolute SHG efficiency is larger than 0.2%) compared to flat areas (Fig. 13b).269
Han et al. proposed that strain is not only a by-product in 2D transfer materials, but also a key means to control the stability and functionality of 2D materials phases.270 They transferred the In2Se3 film onto an uneven substrate, generating controllable local wrinkles, which transformed it from the β phase (ferroelectric) to the α phase (antiferroelectric), thereby enhancing the carrier mobility, improving the on–off ratio and memory performance during the process.
Bubbles, another popular out-of-plane deformation, are prevalent in wet transfer processes.271,272 These microstructures can be deliberately engineered using droplet-assisted transfer. By introducing a water droplet during pick-up, MoS2 can be separated from a hydrophilic SiO2/Si substrate and aligned onto an h-BN layer. Controlled annealing at 130 °C merges small bubbles into larger ones, significantly increasing their aspect ratio and associated local strain. In these bubble regions, PL intensity can be enhanced by more than fourfold, owing to a strain-induced funnel effect that concentrates excitonic energy in the high-strain region.273–275
Beyond strain from direct handling, transferring 2D materials onto rough or patterned substrates can also induce controllable lattice distortions. For example, Ng et al. transferred MoS2 onto a high-roughness, convex substrate by mechanical exfoliation, producing lattice distortion that enhances dielectric screening and suppresses electron–phonon scattering, thereby boosting charge carrier mobility (Fig. 13c).276
Overall, while wrinkles and bubbles are often considered defects, careful engineering of these features, through substrate selection, transfer technique, or post-processing, enables tunable modulation of the mechanical, electronic, and optical properties of 2D materials, opening new avenues for functional device applications—instead of relying on chemical doping, new functions are achieved through mechanical/interface design.
Folding of 2D materials can generally be categorized into two primary strategies: solution-based folding and mechanical folding. In solution folding, liquid-mediated processes, such as selective delamination, capillary action, or surface tension, are employed to induce controlled bending and folding, often with precise control over twist angle and geometry.279,280 For example, solution-based methods can use substrate patterning or interfacial engineering to direct the formation and orientation of folds, enabling the fabrication of tailored structures with unique optoelectronic properties. In contrast, mechanical folding utilizes direct physical manipulation, such as applying a local force with a probe, stamp, or engineered substrate, to bend, fold, or stack 2D layers deterministically. Recent advances in mechanical manipulation have enabled sophisticated 3D operations, such as those demonstrated by Wakafuji et al. using temperature-controlled PDMS/PVC stamps, which permit folding, sliding, rotation, and precise repositioning of 2D flakes (Fig. 14b).281
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| Fig. 14 2D material transfer for folding engineering. (a) The solution-enabled folding: folding of graphene with an arbitrary angle can be achieved using a solution-based method. Reproduced from ref. 284 with permission American Chemical Society, Copyright 2017. (b) The mechanical method for folding: mechanical approaches, such as the AFM probe-based method, can achieve the folding of 2D flakes with arbitrary angles. Reproduced from ref. 281 with permission from American Chemical Society, Copyright 2020. | ||
These folding strategies have been exploited for self-aligned device assembly and multifunctional property modulation. For example, Liu et al. achieved precise alignment in large-area 2D transistors through mechanical folding of graphene/h-BN/MoS2 heterostructures,282 while Zhang et al. used paraffin-induced compression folding (PCF) to introduce strain and enhance photoluminescence in MoS2.283 Additionally, surface engineering methods, such as patterning substrates into hydrophilic and hydrophobic zones, enable further control over folding geometry and twist angle, as demonstrated by Wang et al.284
In summary, both solution-based and mechanical folding approaches provide tunable control over the structure and properties of 2D materials, offering a robust toolkit for engineering novel architectures and multifunctional devices.
One method for realizing and transferring strained 2D materials involves engineering strain prior to transfer. For example, Zhang et al. transferred monolayer strained graphene onto a rigid substrate by initially stretching the graphene on a flexible PDMS support and maintaining a 1.5% tensile strain during transfer.294 To prevent cracking due to stress relaxation, a formalin resin layer was introduced to enhance adhesion and protect the graphene. Buffer droplets on the target substrate provided additional capillary force, facilitating the final transfer of strained graphene. Electrical characterization of back-gated FETs demonstrated increased resistance in strained graphene, attributed to lattice symmetry breaking and altered carrier concentration.295
Strain effects in other 2D materials have also been systematically studied. Conley et al. examined uniaxial strain in monolayer MoS2 by bending the substrate, observing a pronounced decrease in PL intensity under ∼1% strain—signifying a transition from a direct to an indirect band gap.296 Guo et al. further explored strain transfer efficiency by cyclically stretching and relaxing PDMS substrates bearing uniaxially strained graphene.297 Their work highlighted the challenges of maintaining tensile strain, as interfacial slippage can limit the effective transfer, while compressive strain often induces wrinkles, bubbles, or overlaps (Fig. 15a).
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| Fig. 15 Transfer 2D material for strain engineering. (a) The in-plane shear force enabled method.297 The ∼1.5% tensile strain was achieved on a graphene flake by stretching the PDMS substrate. Adapted from ref. 297 according to Creative Commons Attribution 4.0 International License (CC BY 4.0). (b) The out-of-plane force enabled method.298 Tensile strain of a 2D flake can also be achieved by bending the substrate out-of-plane direction. Reproduced from ref. 298 with permission from American Physical Society, Copyright 2009. | ||
Raman spectroscopy provides a sensitive, non-destructive probe of strain in 2D materials, especially through the analysis of phonon modes. Mohiuddin et al. used high-resolution Raman measurements to monitor the photonic response of monolayer graphene under uniaxial strain, observing clear splitting of the G peak into strain-direction-sensitive G+ and G− components, consistent with first-principles predictions.298 These shifts directly reflect changes in lattice constants and phonon energies. Quantification of the Grüneisen parameter and polarization-dependent intensities further enabled mapping of crystallographic orientation and mechanical coupling in graphene devices (Fig. 15b).
Beyond simple mechanical stretching, stress can be engineered to assist in device transfer. Shin et al. demonstrated a dry transfer printing process in which platinum (Pt) films deposited under controlled stress conditions could be selectively detached from the substrate by bending.299 Contacting the strained Pt film with PDMS during substrate bending enabled facile pick-up and flexible device fabrication.
In summary, these approaches illustrate the versatility and promise of strain engineering in 2D materials, not only for tuning electronic, photonic, and optical properties, but also for facilitating new transfer and integration strategies critical for device applications.
In order to study the quantum physics of twist devices, the twist angles should be precisely controlled, because even a slight change in twist angles is adequate to generate a completely new electronic spectrum.109 A smaller twist angle will create a larger Moiré lattice,307 and a “mini-Brillouin zone”. This is the origin of many physical phenomena, such as flat bands and reconstruction of energy band structures, leading to some novel quantum behaviors. For example, unconventional superconductivity,109,308,309 ferromagnetism,310 and Mott-like insulating states311 were found in twisted bilayer graphene (tBLG). Among the other twisted structures, the most common one is stacked and twisted by h-BN and graphene to produce the Moiré superlattice. Since there is a small lattice mismatch between the two materials (δ −1.7%),312 a near-zero twisted angle can significantly change the band structure of graphene, resulting in many interesting phenomena, including the famous Hofstadter Butterfly,110,313–316 Mini Dirac Cone317 as well as the Quantum Hall effect.318 In addition to twisted double layer graphene319 on h-BN, superconductivity and Mott-like insulating states have also been found in three layers of graphene320,321 on h-BN. These fascinating and exotic electronic behaviors are controlled by the modulation of twisted angles.322 In this section, we will focus on the method philosophy for fabricating twist devices. The efficient twist methods to fabricate 2D stacked structures with high quality and precise twist angles will be introduced, including the etching-assisted transfer methods and etching-free dry transfer methods.
The laser assisted cutting-rotation-stacking technique was first proposed by Chen et al. to achieve a high-precision controlled twist angle of 0.1°.303 The detailed preparation process of the laser cutting method is shown in Fig. 16a. Firstly, a PMMA thin film is spin-coated as a supporting layer. Then, a femtosecond laser is used to cut the 2D flake and produce the parallel straight edges, which can be considered as the guideline to precisely control the rotation angles. After the pre-cutting process, two separate pieces of the same 2D flake (noted as layer one and layer two) with a supporting layer are detached from the substrate after etching by an oxide etching solution. Then, layer one is transferred to a new substrate followed by immersing the substrate in acetone to remove the PMMA film above it, while layer two is flipped over and aligned with layer one with an accurate rotation angle. The twisted homojunction with a clean surface can be achieved after a thermal annealing process. The twist angles of the homojunctions can be extracted from the angular difference of the cutting edges. In addition to the laser cutting technique, the AFM tip can also be used to pre-cut the 2D single crystal materials and produce the reference parallel edges.323 One thing that should be noted is that contamination may be introduced between the interface of the stacked structure during the wet etching process. An etching-free dry transfer method would be preferable to create the twist stacked structures after the laser cutting process, that is, one of the separate pieces of the same 2D flake is directly picked up by a polymer stamp and kept stationary, while the other flake on the substrate is rotated by a specific angle, and then a homojunction with a specific twist angle can be fabricated by reassembling the separated 2D flakes.324
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| Fig. 16 Etching-free twisted method. (a) The femtosecond laser cutting method. Twisted bilayer graphene is fabricated by coating graphene with PMMA, cutting it into two parts, and releasing a PMMA/graphene film through etching. One piece is transferred to a new substrate, while the other is inverted and stacked at a controlled twist angle. PMMA removal and annealing yield the final structure. (b) The in-liquid stacking method. The substrate with a 2D flake is cut into half; one half is floated on water and transferred onto the other half by bottom draining, forming a twisted bilayer with a less controlled angle. (c) Edge cutting method: the 2D film is first picked up with a PDMS stamp and split into half by pressing at the substrate edge, leaving one half on the substrate and the other on PDMS. By rotating the PDMS and realigning, the detached half is released back, forming the desired twisted bilayer structure. (d) The tearing and stacking method: a 2D flake on a substrate is cut into two parts. One half is coated with PMMA, etched to release a floating PMMA/2D film, and aligned onto the other half by water drainage. After acetone removal and annealing, the stacked structure forms a twisted bilayer 2D flake at the target angle. (e) The direct growth method for 2D twisted structures. Adapted from ref. 330 according to Creative Commons Attribution 4.0 International License (CC BY 4.0). | ||
A liquid layer separating and stacking method reported by Puretzky et al. similarly requires etching the substrate and transferring the floating 2D flakes supported by a PMMA film,325 as depicted in Fig. 16b. In this strategy, the substrate with the as-synthesized 2D flakes is precut into two parts. Half of the substrate is coated with PMMA, and a floating PMMA/2DM film can be obtained after etching the substrate. Then, the floating PMMA/2DM film is transferred to a funnel filled with DI water, and meanwhile, the other half of the substrate with 2D flakes is transferred to the bottom of the funnel. As the DI water gradually drains, the floating PMMA/2DM film would slowly approach and finally adhere to the bottom substrate when the DI water is completely drained. The twist angle of the homojunction stacked by liquid layer separation can be defined by the intersection angles of the triangles. This method can create a broad range of twist angles without the aid of a microscope. However, this liquid stacking method is typically applicable to the stacking of 2D materials grown by CVD, since it is difficult to precisely locate a specific 2D material or an exact cutting line when cleaving the substrate without microscopic monitoring. Besides, due to the uncontrollable alignment process, it's challenging to ensure a precise twist angle of the stacked structures.
In the past few years, numerous studies on dry peel-off transfer techniques have been carried out.124,127,326 The edge cutting technique reported by Sun et al. is an efficient dry peel-off method to fabricate m·2N stacked layers by only N sequential stacking operations, where m refers to the layer number of the initial 2D material, and N is the stacking rounds.327 The detailed preparation process of the edge cutting method is presented in Fig. 16c. Firstly, the intact 2D flake is covered and picked up by a PDMS film. Then, one half of the 2DM is pressed to the edge of the substrate and separated from the other half after the PDMS supporter being picked up again. A twist stacked structure with a precise twist angle can be attained through aligning the cutting line and restacking the separated flakes. This dry peel-off method is promising for fabrication of high-quality twist devices due to the etching-free process and high-precision angle alignment. Nevertheless, uneven force applied to the PDMS film may result in the fracture of the 2D materials, especially in the case of monolayer or few-layer materials. Besides, different adhesion forces between the 2DM/2DM and 2DM/substrate interfaces may cause wrinkles, or ruptures, or tensile strain within the 2DM as well.
A tear-and-stack technique is another commonly used peel-off technique to fabricate twisted devices with accurate crystal axis alignment. The specific procedures of the tear-and-stack method are displayed in Fig. 16d. The PDMS handle can be prepared by drop-casting the prepolymer mixture of PDMS and a curing agent on a planar PDMS mold. The hardness of the polymer handle can directly affect the contact force. Take an epoxy handle as an example, since the PDMS handle is softer than the epoxy one, so the former handle can achieve weaker contact force.326 The hardness of the PDMS handle can be controlled by regulating the baking time of the prepolymer mixture. After preparation of the PDMS handle, PVA or PPC can be coated on the handle to pick up the h-BN flake. Herein, since the adhesion force between h-BN and other 2D materials is much larger than that between the SiO2/Si substrate and 2D materials, the intact 2D flake will be torn apart and detached from the SiO2/Si substrate due to the strong adhesion force induced by h-BN. Then, the remaining graphene on the substrate can be rotated with a specific angle assisted by a reference rotary alignment mask and picked up by the h-BN with the other torn half of the graphene. Compared with the laser cutting or AFM tip cutting techniques, the tear-and-stack method requires more simplified procedures since the cutting step is omitted. Additionally, the adhesion of the handle can be controlled by coating different adhesive polymers on it, such as poly(bisphenol A carbonate) (PC),324,328 PMMA,326 PVA,329 or PPC.45 Moreover, with the h-BN as the adhesive layer, the cleanliness of the stacking structure can be improved compared to other transferring methods, which require the dissolution of organic polymer support films. However, h-BN cannot be removed after the fabrication of stacking structure with a precise angle, which may not be applicable for the study of chemical reaction on the 2D heterostructures. The dimension of the transferred materials is also restricted by the size of h-BN.
Among all the methods for fabricating twisted devices, the CVD direct growth method can be used to fabricate large-area, high-quality twisted structures with a large range of twist angles. As illustrated in Fig. 16e(I), a one-step reconfiguring nucleation CVD method for growing twisted bilayer MoS2 with a wide range of rotational angles from 0° to 120° has been proposed by Xu et al.330 The growth of a high-quality twisted bilayer MoS2 is achieved by controlling the gas flow rate and the molar ratio of the mixed MoO3/NaCl. The twist angles of the bilayer homostructures can be easily defined by the angular difference between the edges of the triangular monolayer, as depicted in Fig. 16e(II). The optical microscopy images of the as-synthesized twisted bilayer MoS2 are shown in Fig. 16e(III) and (IV). This CVD method can prepare twisted bilayer homostructures with large sizes and a wide range of twist angles. On the other hand, the twist angles are randomly formed during the CVD process, and it's hard to reproduce the twisted structures with specific pre-designed angles.
In summary, we have reviewed several techniques for the fabrication of twisted devices in detail in this section, such as the laser cutting and stacking method, liquid separating and stacking method, peel-off dry transfer methods (i.e., the edge cutting and stacking method and tear-and-stack method), and CVD direct growth method. Different fabrication methods have their own advantages and disadvantages. For example, etching-assisted transfer methods can reduce the damage risk of the 2D materials due to the existence of the supporting layer, while the etching process may induce contamination between the interface of the twist structures. Dry peel-off transfer methods can create stacked structures with a cleaner interface and higher twist accuracy through a simpler operation procedure, but these methods are only suitable for preparation of 2D homo/heterojunctions with small lateral sizes. CVD direct growth methods can prepare large-scale twisted homostructures; however, the twisted angles are random and unpredictable, and the possibility of reproducing the twisted bilayer with specific angles is extremely low. Therefore, an appropriate method should be chosen based on the specific experimental requirements.
Recently, several in situ twist fabrication strategies have emerged. Given their potential significance, we will discuss these developments in detail in the next section.
This lack of reconfigurability presents major limitations for both fundamental research and device prototyping. Each assembled stack is unique, with its own defects, contamination, and interface history, making it difficult to perform variable-controlled studies or reproducibly explore phenomena such as magic-angle superconductivity, moiré minibands, or twist-angle-dependent excitonic effects.332 In practical device development, the inability to “reset” or reuse the same 2D building blocks hinders rapid iteration, multi-functionality, and efficient material usage. The capability to reconfigure, “hot swap,” or adjust layers and contacts would enable tremendous flexibility in next-generation electronics and quantum devices.
Recent advances have begun to address these challenges with the development of reconfigurable transfer methods, techniques that enable not only precise assembly, but also in situ adjustment, disassembly, and realignment of the constituent layers. These approaches make it possible to tune twist angles or registry continuously, dynamically rearrange layer order, or even reverse device fabrication steps. However, many current implementations still rely heavily on polymer support layers, which are difficult to remove completely and often leave behind residues. These residual polymers can severely limit the utility of reconfigured structures, particularly in surface-sensitive applications such as near-field optical microscopy or chemical catalysis, where a pristine, exposed top surface is essential.180,333,334
In this chapter, we review the emerging landscape of reconfigurable transfer technologies. We discuss their fundamental working principles, highlight strategies for minimizing or eliminating polymer contamination, and propose potential routes toward achieving ideal or quasi-ideal reconfigurable transfer. Finally, we explore in situ approaches that extend beyond conventional transfer, enabling dynamic manipulation and on-demand transformation of 2D assemblies for next-generation quantum and optoelectronic applications.
One influential technique, as demonstrated by Tao et al., utilizes atomically flat, high-adhesion polymers such as PVA or PMMA as handling support layers, as shown in Fig. 17a.333 This method enables the full disassembly of fabricated vdW stacks back into their original building blocks, while preserving their structural integrity and allowing subsequent restacking or re-twisting in any desired sequence or orientation. Unlike traditional PDMS- or PPC-based methods, which either lift entire stacks or lack layer selectivity, this polymer-mediated approach offers a much greater control: each 2D layer can be separated, characterized (for example, via AFM or Raman), and then reassembled with deliberate choice of stacking order, contacts, or twist angle. Furthermore, they demonstrated this by reconfiguring a MoS2 device from n-type to p-type operation, or from back-gate to dual-gate architectures, simply by changing the stacking sequence and contact strategy. Even more complex assemblies, such as four-layer floating-gate memories, were split and recombined, enabling a single set of 2D flakes to serve in multiple, entirely different device roles. However, it should be emphasized that in this method a polymer mediator, such as PMMA or PVA, is intentionally retained on the 2D layers, since its presence is essential for manipulation and repeated disassembly. While the dry process minimizes mechanical damage, the exposed surface cannot be accessed until the polymer is removed, which restricts certain applications.
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| Fig. 17 Reconfigurable transfer methods for reconfigurable twist devices. (a) The polymer-handling-layer-enabled reconfigurable transfer method. Disassembling and reassembling to build a twisted vdW structure have been demonstrated. Adapted from ref. 333 according to Creative Commons Attribution 4.0 International License (CC BY 4.0). (b) The PMMA patch-enabled reconfigurable transfer method. The PMMA patch deposited on the top of the sheet is brought into direct contact with PDMS as an operating handle to achieve the purpose of accurately controlling the twist angle between materials. Adapted from ref. 334 according to Creative Commons Attribution 4.0 International License (CC BY 4.0). | ||
Another approach is offered by dynamic twist control, as demonstrated by Yang et al.334 (Fig. 17b). Their approach employs a precision glass slide, a PDMS hemisphere “gel manipulator,” and a pre-patterned PMMA patch to grip and rotate specific layers within a pre-assembled heterostructure, all while observing under an optical microscope. This enables continuous, in situ tuning of the twist angle or lateral registration between layers, without removing the stack from the device substrate. The technique exploits the superlubricity present at incommensurate 2D interfaces, allowing layers to be slid or rotated with minimal force until “locking” at a magic angle is achieved. However, it is important to note that, similar to the disassembly approach, this method fundamentally depends on the use of a PMMA polymer handle for manipulation. The PMMA patch remains attached to the 2D flake throughout the process and cannot be fully removed without compromising the ability to reconfigure the stack. While PMMA handles can be patterned, detached, and reapplied as needed to target different layers or configurations, a thin polymer residue is inevitably left on the manipulated flakes. As such, although the method is highly reproducible and enables dynamic, reversible control of the twist angle, even for ultra-thin or fragile flakes, the presence of polymer limits the accessibility of atomically clean surfaces, which is a critical consideration for certain advanced optical or chemical measurements. Nonetheless, this reconfigurable strategy significantly broadens the experimental capabilities for exploring magic-angle physics, moiré superlattices, and other emergent correlated states, all within a single device platform.
Altogether, these reconfigurable transfer methods represent a major step forward for the field of 2D materials. They fundamentally change device assembly from a one-shot, irreversible process to a flexible and reversible platform, allowing researchers to correct misalignments, optimize stacking sequences and explore a wide range of device architectures using the very same set of 2D components. This versatility enables systematic and variable-controlled investigations, such as studies of twist-angle dependent phenomena or rapid prototyping of multifunctional devices, while minimizing the waste of high-quality 2D flakes, particularly when sourcing flakes with identical properties such as thickness, doping type, and strain. The ability to repeatedly disassemble and reconfigure stacks, combined with the dry, polymer-mediated approach, helps to preserve interfacial quality and device integrity, as demonstrated by AFM, electronic transport, and Raman measurements.333,334 Moreover, these methods are broadly applicable, extending to various families of 2D materials (including graphene, TMDCs, h-BN, and black phosphorus), a range of metals and dielectrics, and even complex multilayer or hybrid device architectures. In situ strategies are especially powerful, offering dynamic, high-resolution access to twist angle control and emergent moiré physics within a single device.
Nonetheless, a significant limitation persists as current reconfigurable transfer techniques still rely on carrier polymers such as PMMA or PVA for manipulation and stacking. These polymers are difficult to fully remove and inevitably leave behind thin residues, limiting the ability to obtain atomically clean, exposed surfaces. This issue is particularly problematic for applications that demand pristine surfaces, such as near-field optical characterization,165,245,249,335,336 surface-sensitive chemical reactions, or catalysis.245,249,337–341 Addressing these challenges will require the development of new, “polymer-free” reconfigurable transfer processes that maintain atomic cleanliness while retaining the flexibility to build, disassemble, and reassemble arbitrary device architectures.
Despite these outstanding obstacles, the advent of reconfigurable transfer technology is already redefining what is possible in 2D materials research and device engineering. For the first time, the device geometry, stacking sequence, and twist angle are all accessible as continuously tunable and reversible parameters. This emerging capability enables systematic experimentation and multifunctional device concepts that were previously unattainable with traditional, static assembly methods and will likely serve as a foundation for the next generation of quantum, photonic, and electronic innovations built from vdW materials.
To bridge this gap, in situ reconfigurable methods have emerged as a transformative next step. These techniques enable direct, real-time manipulation of the twist angle or layer registry within a vdW heterostructure, even after fabrication is complete and the device is wired. Such in situ tuning allows researchers to systematically explore the evolution of electronic, optical, and quantum properties as a function of twist, strain, or lateral displacement. Unlike conventional stacking methods that “lock in” the structure after assembly, in-situ approaches make it possible to dynamically “retune” the same device platform, opening new opportunities for both discovery and optimization.
A leading implementation of this concept uses AFM to physically rotate individual layers within a heterostructure with nanoscale precision. For example, Ribeiro-Palau et al. realized a dynamically adjustable twist angle in an h-BN/graphene/h-BN stack by stacking a prefabricated h-BN flake atop graphene and then rotating the top h-BN layer in situ with an AFM tip (Fig. 18a(I)–(III)).342 This setup enables real-time control over the interlayer twist angle, allowing systematic investigation of how quantum transport and moiré phenomena depend on stacking geometry. Similarly, Yao and colleagues used AFM-based manipulation in h-BN homojunctions (Fig. 18a(IV) and (V)),343 achieving highly tunable SHG responses and revealing “locking” at specific stacking angles due to enhanced interlayer friction.
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| Fig. 18 Method for in situ adjustment of twisted devices. (a) The AFM-based in situ twist protocol. 2D materials are continuously pushed through AFM. The graphene is first placed on top of the h-BN, and then the preformed h-BN structure is transferred to the top of the graphene. Pushing on the topmost h-BN using an AFM rotates the layer and changes its crystal orientation relative to graphene. (I)–(III) The twisting heterojunctions. Reproduced from ref. 342 with permission from The American Association for the Advancement of Science, Copyright 2018. (IV) and (V) AFM image and SHG image of h-BN rotators dialled to different twist angles. Scale bars in (IV) and (V) are 3 µm.343 Adapted from ref. 343 according to Creative Commons Attribution 4.0 International License (CC BY NC 4.0). (b) The quantum twist microscope (QTM). The QTM can allow the in situ twist and measurement of bi-layer graphene. Reproduced from ref. 346 with permission from Springer Nature, Copyright 2023. (c) The MEMS-based twist protocol. (I)–(V) SHG power map of an as-fabricated MEGA2D device with different contact status. (VI) Raman spectroscopy of a MEGA2D h-BN sample when the twisted h-BN flakes are air-spaced by 0.8 µm (up) and in contact (down). Lines with different colours were taken at different twist angles. The dashed lines denote the centre of the E2g peak fit with a Lorentzian. Reproduced from ref. 347 with permission from Springer Nature, Copyright 2024. | ||
Despite the power of these in situ twist methods, the intricate microscopic phenomena at the twisted interfaces of vdW devices often escape conventional characterization. While scanning tunneling microscopy (STM) is effective for probing local electronic properties, it remains limited to single-point measurements and cannot easily capture the spatial evolution of quantum phases or interference phenomena involving multiple tunnelling paths.344,345
To address these limitations, the quantum twist microscope (QTM) was proposed as a conceptual breakthrough (Fig. 18b).346 The QTM utilizes an AFM cantilever functionalized with a vdW heterostructure (e.g., platinum, h-BN, and graphene), which forms an atomically sharp and tunable interface with a second 2D material on a substrate. When the cantilever tip is contacted and rotated with sub-milliradian precision, QTM enables local tunnelling experiments that probe the electronic structure, momentum dispersion, and the presence of electrons in multiple spatial locations—all in one measurement. The strong coupling of wavefunctions at the vdW interface allows direct mapping of both charged and neutral excitation spectra, with simultaneous control over magnetic field, carrier density, and displacement fields. While the capabilities of QTM are extraordinary, its technical complexity and cost currently limit widespread use to only a handful of advanced laboratories.
Most current in situ twist experiments, however, rely on AFM tip manipulation, which necessitates that the top device layer be patterned or engineered to serve as a mechanical handle. To overcome this, Tang et al. introduced a universal MEMS-based actuation platform (MEGA2D, Fig. 18c).347 This system uses microfabricated silicon columns and pyramidal features for precise, chip-integrated rotational and vertical control of stacked 2D materials. Not only does MEGA2D allow for in situ tuning of the twist angle, but it also enables control over interlayer separation via substrate spacers—facilitating studies of both proximity and spatially modulated coupling. This platform also opens new possibilities for systematically investigating additional stacking parameters such as lateral translation, stretch, tilt, and shear, vastly expanding the configurational landscape for 2D materials research.
To promote these technologies from preliminary demonstrations to wider application, the following issues need to be addressed:
High costs: implementing in situ twist requires the use of high-precision AFM equipment. However, in the laboratory, the popularity of high-precision AFM is still very low. Moreover, the new MEMS devices or dedicated QTM systems are very costly, and their maintenance and calibration also require a lot of resources. Modular, small-sized, low-cost MEMS platforms should be developed to promote standardized, reusable sample holders and control firmware, aiming to lower the entry threshold.
Strict operational requirements: the in situ twist technology has strict requirements in terms of alignment and force control, so operators need to have proficient skills. Different operation rates, contact pressures etc. can also cause human-induced deviations, resulting in poor repeatability and large fluctuations in device data. Promoting automated control, standardized processes, etc., addresses the limitations of manual operation.
Bottlenecks in scalability and scale: although the AFM probe method can be extended to a QTM microscope, it cannot meet the requirements of large areas and large scales. MEMS provides a parallel approach, but its compatibility with other fields has not yet been verified. In the future, arrayable MEMS driving devices will need to be developed and rapid twisting solutions to improve efficiency will need to be explored.
As these technologies evolve toward higher precision, automation, and accessibility, they will play an essential role in realizing the full potential of programmable quantum materials and multifunctional devices.
A core technological driver in this transition is the emergence of the all-transfer strategy, a paradigm in which every component of an advanced device, from the active 2D semiconductor layer to metal electrodes, dielectric layers, and even the complete device stack, is assembled by transfer rather than traditional fabrication. This all-transfer approach offers several compelling advantages. Firstly, it bypasses the need for complex lithography, vacuum deposition, and aggressive etching processes, enabling rapid, low-cost, and lithography-free device fabrication—even outside a cleanroom environment. Second, transfer-based assembly minimizes chemical disorder, contamination, strain, and physical damage that often arise from standard fabrication steps, ensuring that the intrinsic quality of each component is preserved throughout the process. Perhaps most crucially, interface quality, especially at the metal–semiconductor junction, is dramatically improved. Transfer-assembled vdW contacts are free from chemical bonding, disorder, and Fermi-level pinning, allowing device performance to approach the fundamental limits predicted by ideal physics. This stands in stark contrast to traditional top-down approaches, where interfacial damage and chemical interactions frequently degrade device behaviour. Collectively, the all-transfer strategy provides new opportunities for scalable, high-quality device manufacturing, paving the way for next generation 2D electronics and optoelectronics.
Beyond improving the contact and interface quality, the all-transfer strategy also unlocks new design freedoms. Metal contacts, high-κ dielectrics, and even pre-patterned 2D layers can be precisely placed or stacked with minimal restrictions, facilitating complex device architectures and 3D vertical integration. This is particularly relevant as the field moves toward monolithic 3D integration, where reducing the physical connection length and stacking multiple functional layers become essential for overcoming scaling bottlenecks.
In this chapter, we provide a comprehensive overview of the all-transfer strategy. We begin by discussing the transfer of individual device components, such as metals and dielectric layers, with an emphasis on their role in interface engineering and their influence on overall device performance. We then turn to transfer-enabled patterning techniques for 2D materials, which offer a lithography-free pathway to large-area and high-resolution device fabrication.
One landmark method, pioneered by Liu et al. involves fabricating metal electrodes of varying work functions on a donor silicon substrate, coating them with a PMMA support, and then physically laminating these metals onto MoS2 layers that have been mechanically exfoliated and prepared with dielectrics. Alignment is achieved under a microscope, and final PMMA removal yields metal–semiconductor contacts that strictly obey the Schottky-Mott rule: the barrier height is determined by the metal's work function, not by interface states or pinning.352 Devices fabricated in this manner achieve electron and hole mobilities close to theoretical limits, offering a decisive demonstration of the advantages of transfer-based vdW contacts.
To scale up and expand the compatibility of this approach, graphene-assisted metal transfer processes have been introduced.353 Here, large-area single-crystal graphene, grown by CVD on Ge(110), serves as a weakly bound, atomically flat support for metals deposited by evaporation. A PVA film is then laminated on top and mechanically peeled off, carrying the metal film nearly defect-free, thanks to the weak vdW interaction at the metal–graphene interface. Once dissolved in water, the metal–PVA film can be transferred to a variety of substrates, including fragile 2D crystals. This process is gentle enough to maintain the integrity of both the metal and the semiconductor, but does rely on the eventual removal of the sacrificial PVA, which can present residue challenges.
Further advances have tackled both the residue problem and process flexibility. For example, vertical metal-assisted vdW integration leverages Bi2O3-assisted CVD to vertically grow single-crystal nanosheets (e.g., Pd, Cu, and Au), which can then be mechanically transferred and used as templates for ALD growth of ultra-thin, uniform high-κ dielectrics (such as Al2O3 or HfO2) without the need for seeding.89 Similarly, hydrogenated diamond substrates offer extremely low adhesion for metal films, allowing for the clean pick-up and transfer of prefabricated metal patterns by PC or PPC stamps.354 These reusable diamond substrates support standard lithography and enable transfer of a wide range of metals, including those difficult to manipulate by conventional dry transfer.
Another innovative route is the ice-assisted in situ transfer, in which a thin layer of amorphous water ice acts as a buffer during metal deposition.355 After the desired metal thickness is evaporated onto the cold sample, the ice is sublimed in a vacuum, causing the metal film to collapse gently onto the underlying 2D material, leaving behind a pristine, undamaged metal-semiconductor interface. This approach also removes adsorbed contaminants, producing a high-quality device interface.
In parallel, high-pressure extrusion methods are pushing the boundaries of 2D metal fabrication. For example, metal powders are melted and pressed between anvils in the presence of monolayer MoS2, yielding atomically flat, large area (>100 µm) 2D metals that can be mechanically exfoliated and encapsulated for further studies.226 Such contacts are inherently non-bonding, minimizing gap states and maximizing surface smoothness, with physical isolation inhibiting metal-induced gap states (MIGS) and reducing Fermi level pinning.
Each of these methods, including physical lamination, graphene or diamond-assisted transfer, ice buffering, and vdW extrusion, highlights the importance of achieving clean, residue-free, and atomically precise interfaces in 2D device engineering. The formation of van der Waals metal-semiconductor contacts enable the Fermi level to align closely with the work function of the selected metal, thereby avoiding the interfacial disorder and electronic traps that often limit the performance of conventional contacts.
Nevertheless, practical challenges remain. The mechanical transfer process can introduce non-uniformities at the vdW interface, leading to local tunnelling barriers and increased contact resistance. In addition, sacrificial layers (PMMA and PVA) may leave behind residues that, if not carefully managed, could degrade device performance. Continuous improvement in transfer media, alignment strategies, and cleaning protocols will be crucial for the widespread adoption of these techniques in high-yield, wafer-scale device manufacturing.
2D semiconductors, with their atomically thin profiles and inherent surface passivation, offer a compelling alternative. Their strong quantum confinement effectively suppresses short-channel effects and leakage current, enabling enhanced gate control. However, the integration of high-quality, ultrathin dielectric layers onto 2D materials presents its own set of challenges. Traditional ALD processes rely on surface chemical activity, which is often absent on inert 2D crystals and therefore necessitates the use of seeding or nucleation layers. These seed layers, while enabling dielectric growth, can introduce defects or “dangling bonds” that degrade interface quality and device mobility.
To circumvent these issues, the transfer of prefabricated, high-quality dielectrics using a vdW integration approach has emerged as a transformative solution. In this process, crystalline or amorphous dielectric films (e.g., Al2O3, HfO2, Y2O3) are first grown on sacrificial substrates (often buffered by a polymer or graphene interlayer), then picked up and laminated directly onto the 2D semiconductor via dry or wet transfer. This bypasses the need for nucleation on the channel surface, preserves atomic flatness, and creates a clean vdW gap at the interface, effectively reducing interface states and suppressing gate leakage. The presence of a few-angstrom-wide vdW gap further mitigates edge-induced barrier lowering and minimizes gate-induced carrier tunnelling, yielding superior gate control and device performance.
Several advanced protocols have been developed to realize these goals. For instance, Lu et al. introduced a dry dielectric transfer strategy, in which Al2O3 or HfO2 is deposited atop a thin PVA buffer layer on silicon, then etched and laminated onto wafer-scale monolayer MoS2 via heat-releasable tape and mild plasma treatment.88 This ensures atomic flatness and preserves surface cleanliness, with the thin PVA enabling subsequent ALD growth of uniform dielectrics.
Other innovations exploit graphene as a sacrificial buffer. Wang et al. deposited Y2O3 atop graphene on SiO2, then annealed and oxygenated the film to form atomically flat Y2O3.358 The structure is supported by PMMA, then the graphene is removed by plasma etching, and the dielectric is transferred to the device. Inheriting the flatness of graphene, this “one-step lamination” method enables the integration of complex device stacks onto arbitrary substrates.
While amorphous oxides such as SiO2, Al2O3, and HfO2 can effectively reduce leakage, they often harbour a high density of interface defects due to their structural disorder. To address this, researchers are exploring single-crystal dielectric materials, such as h-BN and CaF2, which provide atomically smooth, lattice-matched interfaces and minimal defect densities. However, even ultra-thin h-BN may show high leakage at nanoscale thickness, motivating the search for new high-κ, large-band-gap crystalline dielectrics.
Recent breakthroughs include the use of perovskite oxides and single-crystal films. For example, ultrathin, transferable SrTiO3 (STO) has been realized by growing STO on a water-soluble sacrificial Sr3Al2O6 layer, supporting it with PDMS and then dissolving the sacrificial layer to release atomically flat STO for transfer.359 Such single-crystal films achieve dielectric breakdown fields and low leakage comparable to or exceeding amorphous counterparts, though current implementations are mostly limited to back-gate FET architectures.
In another advance, layered perovskite oxides such as Sr2Nb3O10 (SNO) have been assembled via Langmuir–Blodgett techniques or top-down liquid-phase exfoliation and then transferred using polymer stamps to form heterostructures.360 These crystalline dielectrics offer high-κ, robust band gaps, and atomically sharp interfaces, resulting in FETs with steep subthreshold swings and high on/off ratios.
Furthermore, emerging ferroelectric dielectrics, such as transferred Hf0.5Zr0.5O2 (HZO) films, enable integration of non-volatile memory and logic into 2D architectures, with recent work demonstrating wafer-scale transfer and high-yield device performance.361
In summary, transfer-based integration of high-κ dielectrics with 2D materials, via vdW lamination, crystalline oxide exfoliation, or sacrificial-buffer techniques, provides a pathway to ultra-scale, low-leakage, high-mobility devices. The approach overcomes the limitations of direct ALD or CVD growth, enabling the construction of pristine interfaces, minimizing defect densities, and expanding the palette of available dielectrics. As the toolkit for dielectric transfer expands, the prospects for all-transfer, wafer-scale, and three-dimensional integration of 2D devices become ever more promising, accelerating progress toward next-generation electronics and quantum technologies.
The process begins by fabricating and patterning a large array of 2D devices (such as transistors, photodetectors, or logic gates) on a growth or donor substrate using established techniques. Once the devices are completed, a support layer (typically a polymer film) is laminated onto the surface. The underlying sacrificial substrate is then selectively etched or dissolved, releasing the entire device array, which can be picked up and precisely transferred to a target wafer or even stacked onto another 2D device layer (see Fig. 19c).
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| Fig. 19 All transfer strategies. (a) Transfer metal.356 (I) Printing metal patterns on the target substrate. (II) The inset shows an optical image of the transferred Au pattern array. Reproduced from ref. 356 with permission from Springer Nature, Copyright 2022. (b) Transfer dielectrics. (I) Pre-deposition on a PVA sacrificial layer using the ALD process. (II) Dielectric dry peeling-off. (III) Dielectric lamination on top of a target substrate. Adapted from ref. 88 according to Creative Commons Attribution 4.0 International License (CC BY 4.0). (c) Transfer device. (I) Optical images of a prefabricated circuit tier on a 2-inch sacrificial substrate. (II) The zoomed-in image. (III) The optical image of the final device fabricated by laminating the circuit tier onto an MoS2 substrate; the top patterned MoS2 channel is highlighted by a red dashed box. (IV) The corresponding optical image of the 10-tier M3D systems. The MoS2 substrates are grown using chemical vapour deposition within the 10-tier integration. Reproduced from ref. 357 with permission from Springer Nature, Copyright 2024. | ||
Crucially, this approach decouples fabrication from integration: devices can be batch-produced under ideal growth and patterning conditions and later reconfigured, relocated, or stacked as needed. The advantages are multifold: (1) fabrication efficiency, through modular and scalable assembly; (2) stacking and heterogeneous integration, enabling monolithic 3D logic, memory, and sensing architectures; (3) damage-free assembly, since no erosive processing is imposed post-transfer; and (4) substrate versatility, allowing integration onto flexible, transparent, or bio-compatible platforms. Liu et al. showcased the transformative potential of van der Waals (vdW) lamination as a low-temperature route to monolithic three-dimensional (M3D) integration (Fig. 19c(I)–(IV)).357 By sequentially stacking entire prefabricated circuit layers, they realized a ten-tier vertical M3D system. Remarkably, the vdW-mediated process confined the integration temperature to only 120 °C—well below the thermal budget restrictions that undermine conventional silicon-based M3D integration and hinder its compatibility with back-end-of-line (BEOL) processes. Equally critical, vdW transfer circumvents the need for harsh lithography or etching directly on 2D lattices, thus preserving atomic integrity while maintaining device performance. In parallel, Tao et al. demonstrated that prefabricated MoS2 transistors could be laminated onto vertical stacks using a T-shaped PDMS stamp, achieving a 60-device array without degradation.362 This strategy effectively overcame the inherent planar constraints of conventional lithographic processes, bridging lateral device fabrication with vertical stacking and thereby expanding the dimensionality of integration.
In summary, the transfer of whole 2D devices represents the next logical step in the all-transfer strategy. By enabling modular, reconfigurable, and damage-free assembly of complex electronic and optoelectronic circuits, it holds great promise for future wafer-scale integration, high-density logic and memory, and novel multi-functional device concepts. As transfer protocols mature, fully transfer-based device engineering may become the foundation for future electronics beyond the limits of traditional top-down fabrication.
Direct pattern transfer has thus emerged as a transformative solution, enabling the deterministic patterning and integration of 2D materials entirely without photolithography, masks, or solvents (Fig. 20). This paradigm shift is underpinned by several innovative approaches, each with its own unique technical merits and challenges.
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| Fig. 20 Photolithography-free pattern transfer. (a) The water-assisted wafer-scale transfer printing technology. Reproduced from ref. 133 with permission from Springer Nature, Copyright 2025. (b) The adhesive matrix transfer method for wafer-scale patterned 2D material integration. Reproduced from ref. 363 with permission from Springer Nature, Copyright 2023. (c) The direct metal stamping method for wafer-scale fabrication. Reproduced from ref. 364 with permission from Springer Nature, Copyright 2025. | ||
A pioneering strategy is the MTP technique developed by Zhou Peng's group (Fig. 20a).133 Here, a PDMS stamp patterned with an array of microcolumns is used to selectively contact and retrieve 2D materials from a growth substrate. During the process, a capillary-active mixed solution (ethanol/water) infiltrates the interface between the PDMS stamp and the substrate, enabling selective pick-up of contacted regions via capillary peeling. Subsequent alignment and mild heating allow the patterned 2D material array to be released onto the target substrate with high spatial precision. This method has been used to deterministically transfer 2-inch-scale monolayer MoS2 arrays, achieving over one million functional devices per wafer, all while retaining their pristine electrical performance. MTP elegantly bypasses resist processing and chemical etching, making it exceptionally attractive for large-area, contamination-free 2D device fabrication. However, a critical bottleneck remains: the lateral resolution is fundamentally limited by the mechanical deformability of the PDMS microcolumns. As device dimensions approach the deep submicron regime, further progress will hinge on the development of stiffer, less deformable stamps or hybrid mechanical structures. Nevertheless, the high yield, process simplicity, and compatibility with scalable CVD-grown films render MTP a promising candidate for industrial 2D electronics.
To overcome the force limitations intrinsic to van der Waals pickup, adhesive matrix transfer has been developed by Farnaz Niroui's team (Fig. 20b).363 In this approach, the receiving substrate (such as SiO2) is embedded in an adhesion-tunable matrix (e.g., patterned gold), enabling selective, high-strength interaction with the 2D material of interest. Unlike vdW stamping, the matrix can overcome weak interfacial adhesion, ensuring residue-free pickup and transfer of even the most challenging materials. This method enables one-step device integration, supports complex patterning, and preserves ultra-clean, exposed surfaces essential for subsequent functionalization or advanced quantum devices. Adhesive matrix transfer stands out for its exceptional interface cleanliness and its ability to break through vdW force limits. Notably, it eliminates the need for solvents, sacrificial layers, or thermal steps, thereby preserving the atomic flatness and electronic structure of transferred films. However, the method currently relies on precise matrix engineering for each material, and its extension to highly heterogeneous or flexible substrates is an open technical question. Nevertheless, the single-step process and mask-free patterning make it a valuable addition to the 2D device fabrication toolbox.
Recently, Li, et al. introduced a lithography-free patterning strategy by direct metal stamping (Fig. 20c).364 Here, a pre-designed 3D metal stamp is pressed onto a continuous 2D material. Owing to the strong local metal-2D material interaction, only the contact regions are picked up, while the non-contact areas remain on the growth substrate, resulting in cleanly patterned 2D arrays. The resulting devices, fabricated without any photoresist or chemical reagents, exhibit high performance and remarkable uniformity across large scales. This strategy is remarkable for its complete elimination of chemical patterning steps and post-transfer processing, offering the highest attainable cleanliness and structural integrity for 2D arrays. The main limitation lies in the design, cost, and reusability of the metal molds, especially for complex or fine-feature arrays. Future improvements in scalable, reconfigurable mold design could further enhance the practicality of this approach for industry.
In addition, a diverse suite of transfer-enabled, lithography-free patterning techniques, such as water-assisted transfer printing, single-lamination stacking, and one-step vdW integration, have rapidly expanded the design space for 2D devices and circuits. These methods enable high-yield, contamination-free fabrication across both planar and vertical architectures, support a wide range of substrates (including flexible and unconventional platforms), and deliver atomic interface quality unattainable by conventional lithography. While each approach has unique strengths and current technical limits, together they redefine scalable manufacturing in 2D electronics and bring modular, industrial-level device integration within reach.
In summary, transfer-enabled, lithography-free patterning is fundamentally redefining device manufacturing in 2D electronics. By circumventing the limitations of traditional photolithography and wet processing, these methods deliver new levels of scalability, yield, and interface quality for both planar and vertical device integration. As each approach continues to mature, a hybrid toolbox combining pattern transfer, adhesive engineering, and vertical stacking will likely emerge, paving the way for modular, high-performance, and industrial scale 2D electronics with truly clean and tunable interfaces.
A notable example is provided by Yu et al., who applied a deterministic dry transfer process to fabricate twisted bilayer graphene (TBG)/h-BN heterostructures with precisely controlled twist angles.24 This approach revealed an unambiguous correlation between moiré geometry and interfacial electron-transfer kinetics: electrochemical measurements showed that reaction rates are maximized near the “magic angle” (∼1.1°), where flat-band states localise carriers and amplify electronic density of states (Fig. 21a). This discovery positions the twist angle as a controllable degree of freedom for electrochemical reactivity, circumventing the stochasticity of dopant incorporation or defect engineering. Subsequent work extended this moiré-reactivity paradigm to transition metal dichalcogenides (TMDs), underscoring its potential impact on photoelectrochemistry and electrocatalysis, where band structure-driven reactivity tuning could complement or even supplant conventional catalyst modification strategies.
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| Fig. 21 Applications of 2D materials in other fields. (a) Chemistry. Reproduced from ref. 24 with permission from Springer Nature, Copyright 2022. (b) Tribology and haptics. Reproduced from ref. 27 with permission from American Chemical Society, Copyright 2023. Reproduced from ref. 28 with permission from Wiley-VCH, Copyright 2016. (c) Thermal transport and thermodynamic control. Reproduced from ref. 29 with permission from American Chemical Society, Copyright 2021. Reproduced from ref. 30 with permission from Elsevier, Copyright 2024. | ||
Equally transformative is the application of twist-controlled stacking to two-dimensional covalent organic frameworks (2D COFs), whose extended π-conjugation and tunable pore architectures make them attractive for catalysis, sensing, and energy storage.291 Conventional COF synthesis typically yields rotationally disordered stacks due to the near-isoenergetic nature of different twist configurations, resulting in heterogeneous interlayer coupling. Recent advances, exemplified by Zhan et al., have addressed this by directly synthesising bilayer COFs at a liquid–substrate interface under conditions that promote deterministic stacking control.365 Through monomer structure design and mixed-solvent modulation, which can balance precursor solubility with low volatility, the authors achieved large-area moiré superlattices with a predominant twist angle (∼9.2°) verified by atomic-resolution HRTEM and reciprocal-space mapping. This breakthrough not only extends moiré engineering beyond van der Waals solids into covalent molecular architectures, but also unlocks new opportunities to modulate electronic coupling, exciton dynamics, and host–guest chemistry through precise stacking symmetry control.
In summary, these studies exemplify how transfer-enabled twist engineering is evolving from a structural curiosity into a chemically actionable variable—capable of bridging solid-state physics and synthetic chemistry to create functional interfaces with unprecedented precision. Looking forward, integrating in situ spectroelectrochemical probes, operando microscopy, and theory-guided twist-angle selection could yield predictive control over reactivity landscapes, accelerating the design of catalytic, photochemical, and sensing platforms based on moiré-tailored 2D materials.
More recent work has explicitly connected these effects to moiré superlattice engineering. Liu et al27 showed that graphene grown on Pt exhibits moiré patterns due to partial lattice mismatch (Fig. 21b(I)–(III)) and that adjusting the twist angle allows for reversible switching between dissipative sliding and ultra-low-friction states. Here, both the moiré periodicity and the normal load threshold govern the transition: below the threshold, the interface remains in a constant superlubric state, while above it, the friction coefficient decreases systematically with increasing moiré period. These findings are supported by theoretical models linking twist-induced modulation of in-plane and out-of-plane deformation fields to energy dissipation pathways.
In the field of haptics, the exceptional thinness, mechanical compliance, and electromechanical sensitivity of 2D semiconductors have inspired a new generation of tactile sensors. Park et al28 fabricated strain-gauge sensors based on monolayer MoS2, achieving high gauge factors (GF), optical transparency, and mechanical flexibility (Fig. 21b(IV)–(VIII)). Devices maintained high sensitivity, uniformity, and linearity after 10
000 bending cycles, and their ∼75 nm total thickness allows direct integration onto non-planar and even skin-mounted substrates. These attributes make 2D-based tactile sensors attractive for wearable electronics, human-machine interfaces,368–370 and prosthetic feedback systems.371,372
Twist engineering in vdW heterostructures offers a powerful route to modulate phonon transport, providing a thermodynamic handle for heat management in nanoscale devices. By altering the interlayer registry, the twist angle can directly influence phonon spectra, scattering pathways, and mode coupling—parameters that govern both in-plane and cross-plane thermal conductivity.
Ren et al. demonstrated that in graphene/h-BN bilayers, the in-plane thermal conductivity decreases monotonically, by up to 50%, as the twist angle increases from 0° to 30° (Fig. 21c(I) and (II)).29 This reduction was attributed to enhanced surface corrugation, which amplifies low-frequency (<10 THz) phonon scattering and suppresses interlayer phonon transmittance. Such a strong angular dependence reveals that even modest misalignment can be used to deliberately tune heat dissipation in vdW devices.
Extending this principle to hybrid heterostructures, Meng et al. employed non-equilibrium molecular dynamics (NEMD) simulations to study graphene/MoS2/graphene stacks at varying twist angles (Fig. 21c(III) and (IV)).30 They found that the in-plane thermal conductivity of the MoS2 layer drops sharply with increasing twist angle, reaching a minimum at 10.893°, where it is only 47.3% of the untwisted value. This degradation stems from twist-induced lattice mismatch, which produces uneven stress fields and enhances phonon–phonon scattering. Interestingly, they also observed that increasing the number of graphene layers reduces the interfacial thermal resistance, as additional layers mitigate out-of-plane atomic displacement and improve structural stability.
In parallel, Ouyang et al. examined uniformly twisted graphite and h-BN multilayers, finding that the interfacial thermal resistance (ITR) increases markedly with the twist angle.31 This behavior arises from reduced phonon mode coupling at misaligned interfaces, thereby lowering cross-plane thermal conductivity. Such control over interfacial thermal isolation is particularly relevant for applications requiring thermal shielding between an active layer and its substrate.
In summary, these studies position the twist angle as a versatile thermodynamic tuning parameter, enabling thermal conductivity suppression, directional heat management, and interfacial thermal isolation in 2D-based devices. By leveraging twist-induced phonon engineering, it is possible to co-optimize thermal transport with other functionalities such as friction modulation, mechanical stability, and optoelectronic performance.
One of the most striking phenomena accessible via twist engineering is the photonic “magic angle”, a rotation configuration where the PhP isofrequency contours flatten, entering the canalization regime.377,378 In this state, polaritons propagate in a highly collimated, unidirectional manner with negligible geometric spreading, enabling sub-diffractional information transport over extended distances.379,380 The canalization direction and wavelength are uniquely determined by the magic angle and material thickness, making twist control central to device functionality.381
α-Phase molybdenum trioxide (α-MoO3), a naturally hyperbolic vdW crystal, provides an ideal platform for such studies due to its strong in-plane anisotropy and the ability to achieve clean rotational interfaces via all-dry viscoelastic stamping. Hu et al. demonstrated a topological transition of PhP dispersion in twisted bilayer α-MoO3, tunable from hyperbolic to elliptical regimes by adjusting the rotation between layers along crystallographic [001] or [100] axes (Fig. 22a).25 For a given frequency, only a single photonic magic angle exists, which confines canalization to a narrow set of directions and restricts all-angle tunability in bilayer geometries.
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| Fig. 22 Twist for optical devices. (a) Polariton dispersion is controlled by twisted bilayered α-MoO3. Reproduced from ref. 25 with permission from Springer Nature, Copyright 2020. (b) Photonic magic angles and polariton canalization in reconfigurable trilayers. Reproduced from ref. 26 with permission from Springer Nature, Copyright 2023. | ||
To overcome this constraint, Duan and co-workers introduced a reconfigurable twisted trilayer α-MoO3 architecture (Fig. 22b).26 Fabricated via sequential PDMS-assisted stacking of exfoliated α-MoO3 flakes, the device features two independently set twist angles—θ1–2 (bottom-middle) and θ1–3 (bottom-top)—which can be reprogrammed by layer disassembly and reassembly. Near-field scanning optical microscope (s-SNOM) and full-wave simulations (Fig. 22b(I)–(IX)) revealed multiple photonic magic angles within a single device: for θ1–2 = 30°, canalization directions of 140°, 80°, and 50° were achieved at θ1–3 = −90°, −60°, and −40°, respectively. This multi-angle flexibility enables broadband canalization and all-directional polariton steering within the device plane—capabilities unattainable in bilayers. Importantly, these properties persist across a wide spectral range and for varying layer thicknesses, underscoring their robustness.376
By unlocking deterministic control over polaritonic dispersion, twist-engineered α-MoO3 heterostructures open new frontiers for mid-IR nanophotonics, including compact waveguides, reconfigurable beam steering devices, and ultra-thin hyperlenses.183 The ability to combine dry-transfer precision, multiple rotational degrees of freedom, and broadband robustness marks a significant step toward programmable polaritonic circuitry.
Beyond intrinsic nonlinear properties, symmetry engineering has emerged as a powerful approach. Zhang et al. reported emergent SHG in otherwise centrosymmetric bilayer MoS2 when stacked with monolayer graphene.344 Interlayer charge transfer broke the inversion symmetry of MoS2, producing SHG of comparable strength to monolayer MoS2. This effect—absent before interlayer coupling was established—illustrates how charge transfer in van der Waals heterostructures can be exploited to tailor nonlinear optical responses and potentially activate SPDC processes in systems previously deemed inactive.
Control of nonlinear wave mixing can also be achieved via nonlinear geometric phase engineering. Hong et al. showed that twisting multilayer films by an optimal angle can induce a geometric phase that compensates phase mismatch, enabling high SHG conversion efficiencies (∼8% in 3.2 µm-thick stacks) and tunable output polarization383 (Fig. 23a(I)–(III)). The “Twist-PM” concept aligns the SHG contribution vectors from each layer to achieve constructive interference, offering a route to polarization- and phase-controlled quantum light emission in ultrathin platforms. In parallel, another twist stacking quasi-phase-matching strategy has been adapted to 3R-MoS2. Tang et al. demonstrated that 3R-MoS2 stacks with controlled 60° rotational offsets between successive layers create periodic modulation of the nonlinear polarization along the growth axis, surpassing the non- quasi-phase matching (QPM) SHG limit(Fig. 23a(IV)–(VI)).384 Such QPM structures are promising for enhancing SPDC efficiency in atomically thin materials, enabling brighter entangled photon pair generation in ultracompact geometries.
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| Fig. 23 (a) Twist phase matching. (I)–(III) The nonlinear geometric phase caused by the twist angle is used to compensate for the phase misfit in the SHG process. Reproduced from ref. 383 with permission from American Physical Society, Copyright 2023. (IV)–(VI) Theoretical model of a unique QPM enabled by van der Waals stacking. Adapted from ref. 384 according to Creative Commons Attribution 4.0 International License (CC BY NC ND 4.0). (b) Periodically poled layered semiconductors. (I) and (II) The quasi-phase-matched frequency conversion enabled by the χ2 sign flip.385 Reproduced from ref. 385 with permission from Springer Nature, Copyright 2025. | ||
The concept of periodic poling, which is well established in nonlinear bulk crystals such as periodically poled lithium niobate (PPLN), has recently been translated into the realm of 2D materials, enabling unprecedented control over light-matter interactions at the atomic scale. In a landmark demonstration, Trovatello et al. realized periodically poled transition metal dichalcogenides (PPTMDCs) by fabricating multi-layer stacks of 3R-MoS2 with alternating crystallographic orientations, which periodically invert the sign of the χ2 along the stacking direction to implement QPM in an atomically thin platform (Fig. 23b).385 This architecture supports both up-conversion SHG and SPDC with efficiencies far exceeding the non-QPM limit, and the phase mismatch between interacting waves can be precisely cancelled by tuning the thickness and periodicity of the 3R-MoS2 domains. The monolithic 2D structure minimizes optical loss and allows seamless integration with photonic and quantum devices, offering a route to compact, chip-scale sources of entangled photons and wavelength-tunable light.204,386 This atomically engineered periodic poling approach bridges bulk-crystal nonlinear optics and van der Waals nanophotonics, marking a decisive step toward scalable quantum photonic circuitry based on layered materials.
Taken together, these advances, from giant χ2 2D ferroelectrics like NbOX2174,220,269,382 to symmetry-breaking heterostructures and twist- and QPM-engineered stacks, mark a pivotal step toward ultrathin, chip-integrable quantum photonic devices. The convergence of high nonlinearity, scalable thickness response, and engineered phase matching points to a future where deterministic entangled photon sources and reconfigurable quantum modulators are realized entirely within the van der Waals materials platform.
Since almost all atoms of 2D materials are exposed on the surface (or interface), this increases the coupling efficiency with electric fields, ions, or light, enabling small external fields to effectively modulate parameters such as device conductance/capacitance; this is the key to achieving low energy consumption and adjustable synaptic weights. Many 2D materials support fast electronic transport and reversible ion migration (e.g., metal cations or protons) via defects, adsorption sites, or interlayer channels. This mixed ionic-electronic conduction provides the physical basis for synaptic behaviors: transient ionic redistribution gives rise to short-term plasticity (STP), whereas cumulative/partly irreversible ionic or electrochemical changes underpin long-term plasticity (LTP).387 Furthermore, through factors such as layer thickness, phase transition, defect doping or strain, the conductive/electronic band structure of 2D materials can be controllably adjusted, thereby achieving multi-level tunable conductance levels. This is one of the core functions required by neuromorphic hardware.388
For instance, Qin et al. developed a molecular crystal memristor. The representative channel material Sb2O3 has a molecular crystal structure, in which the molecular cages are interconnected through van der Waals forces.389 This unique structure enables ions to migrate through the molecular gaps with relatively low energy input, maintaining the integrity of the crystal structure even after numerous switching cycles. The energy consumption for a single operation is as low as 26 zJ. It completed 109 cycles and successfully fabricated a large cross-array on an 8-inch wafer, while also achieving single-chip integration with CMOS technology, demonstrating its significant industrialization potential. Teja Nibhanupudi et al. reported ultrafast memristors fabricated using 2D h-BN. They synthesized few-layer h-BN on copper foil using the CVD method and transferred it onto a Si/SiO2 substrate to fabricate the memristors. The switching speed reached 120 ps, and the switching energy was extremely low, at 2 pJ.390
Looking ahead, moving from device demonstrations to system-level neuromorphic computing with 2D materials will require cross-layer co-design rather than merely “better heterostructures.” At the materials level, vdW stacks must be engineered to deterministically gate ionic pathways and barriers, enabling on-demand switching between volatile and non-volatile responses while enhancing device stability and uniformity. At the architecture level, scalable three-dimensional integration of 2D devices requires addressing challenges related to endurance, retention, and transfer interfaces, as well as achieving ultra-low energy consumption at the system level rather than for individual devices. These advances will ultimately enable the realization of biologically realistic neural networks comprising synapses, dendrites, and somas, fully integrated within compact on-chip systems.
Bae et al. developed a R2R transfer process for large-area graphene films, using them as transparent electrodes, laying a feasible path for large-area flexible energy storage devices.200 Zhu et al. placed a single layer of MoS2 on a conductive substrate (graphene/gold film) through a transfer process to form an electrocatalytic electrode and investigated the role of the boundary activation effect in the hydrogen evolution reaction.33 In this study, the transfer engineering ensured that the large-area single-layer MoS2 could serve as an actual electrocatalytic electrode. Park et al. coated the surface of high-nickel cathode particles with graphene layers, significantly reducing the reliance on conductive agents and binders. Graphene sheets were uniformly covered on the surface of the cathode particles through transfer/coating processes. This enhanced the volumetric energy density and cycle stability of the battery.34
For 2D materials to truly enter the field of energy applications, several issues need to be addressed, including large-scale controllable fabrication and transfer, long-term stability, and device-level integration. By developing low-cost, scalable synthesis and transfer methods, combined with interface and defect engineering, heterostructure design, and intelligent simulation and prediction, it is expected to achieve precise control over performance. At the same time, by further expanding 2D materials into new energy systems such as solid-state batteries and photocatalytic hydrogen production, it is possible to drive a qualitative leap in energy storage and conversion technologies (Fig. 24).
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| Fig. 24 (a) Neuromorphic computing. (I) and (II) Schematic of the molecular crystal memristor in the crossbar array architecture. Reproduced from ref. 389 with permission from Springer Nature, Copyright 2025. (b) Electrocatalysts. (I) The nonlinear geometric phase caused by the twist angle is used for high density of domain and phase boundaries. Adapted from ref. 33 according to Creative Commons Attribution 4.0 International License (CC BY 4.0). (c) Energy. (I)–(IV) Schematic structure of the multi-hierarchy MoS2 catalysts. Adapted from ref. 34 according to Creative Commons Attribution 4.0 International License (CC BY 4.0). | ||
Nevertheless, several grand challenges remain. Cleanliness and interface control continue to be the most critical bottlenecks. Conventional polymer-assisted protocols inevitably leave residues or interfacial defects that compromise transport and optical performance. Emerging concepts such as sacrificial mediator layers, intrinsically clean dry transfer, and dynamically tunable adhesion present promising solutions, but a universal, residue-free transfer process remains elusive. Equally urgent is the need for reconfigurability: current methods largely enable static stacking, whereas future directions should aim at reversible and in situ manipulation of twist angle, spacing, and domain registry. Such capabilities would open programmable device architectures, where 2D heterostructures can be dynamically tuned post-integration.
Scaling toward wafer-level integration is another frontier. While proof-of-concept demonstrations of large-area printing, stamp patterning, and R2R assembly exist, the uniformity, throughput, and CMOS compatibility remain limited. The convergence of robotics-assisted transfer, real-time metrology, and advanced adhesion engineering will be essential to bridge laboratory methods with industrial fabrication, ultimately enabling defect-free integration on 200–300 mm wafers. In parallel, in situ transfer concepts, where growth and relocation are integrated into continuous workflows, may eliminate stochasticity and reduce contamination, offering a seamless path to twist-controlled and multilayer heterostructures.
Looking forward, the scope of 2D transfer technology will extend beyond conventional electronics and photonics. Applications in tribology, haptics, wearable devices, chemistry, and thermal management are emerging, where controlled interfaces and ultrathin integration provide unique functionalities. Notably, twist-phase-matching and periodically poled 2D crystals point to a paradigm shift in nonlinear optics, enabling frequency conversion and quantum light generation in atomically thin platforms. Extending such concepts to wafer-scale, reconfigurable devices would open a new class of integrated nanophotonic and quantum technologies. Beyond these areas, the integration of ultraclean and reconfigurable 2D heterostructures may also provide decisive advantages for quantum computing, where atomic-scale control of interfaces and twist-dependent quantum phases can be harnessed to engineer qubits, quantum interconnects, and scalable architectures.
In conclusion, the future of 2D transfer lies in developing methods that are intrinsically clean, dynamically reconfigurable, and scalable to wafer-level integration. Achieving these milestones will not only overcome existing bottlenecks but also elevate transfer technology from a fabrication tool to a discipline in its own right, bridging chemistry, physics, and engineering while unlocking the full potential of low-dimensional materials in next-generation technologies.
The analyses are available within the supplementary information (SI). Supplementary information is available. See DOI: https://doi.org/10.1039/d5cs00531k.
Footnote |
| † Co-first authors. |
| This journal is © The Royal Society of Chemistry 2026 |