Open Access Article
Hyo Jong Choa,
Jun Yong Kima,
Ki Won Jeonga,
Soo-Hwan Jeong
*bc and
Yun Seon Do
*a
aSchool of Electronic and Electrical Engineering, Kyungpook National University, Buk-gu, Daegu, 41566, Republic of Korea. E-mail: yuns.do@knu.ac.kr
bDepartment of Chemical Engineering, Kyungpook National University, Buk-gu, Daegu, 41566, Republic of Korea. E-mail: shjeong@knu.ac.kr
cSchool of Chemical Engineering and Applied Chemistry, Kyungpook National University, Buk-gu, Daegu 41566, Republic of Korea
First published on 27th October 2025
Conventional dye-based color filters suffer from limited chemical stability and environmental durability. Structural color technologies that exploit nanophotonic phenomena offer a promising alternative; however, fabricating intricate nanostructures and multicolored patterns over a large area remains a significant challenge. Here, we present a scalable approach to artwork-like coloration by using spatially patterned anodic aluminum oxide (AAO) as the dielectric layer in metal–insulator–metal (MIM) cavities. Local modulation of the anodization conditions on a single aluminum film allows precise engineering of the effective refractive index values of the AAO layer. This introduces a conceptual shift: resonance is decoupled from geometrical factors and governed instead by porosity-driven refractive index modulation, a new design lever for nanophotonics. Consequently, diverse color domains are generated within a single cavity profile, enabling planar integration. Artwork-like multicolor patterns with aesthetic and functional impact are achieved on centimeter-scale substrates, and, because anodization is already an industrially established large-area process (used even in aircraft components), the method is inherently scalable to much larger surfaces.
New conceptsThis work introduces a new paradigm for structural coloration by decoupling optical resonance from geometrical parameters and exploiting porosity-driven refractive index modulation in anodic aluminum oxide (AAO). Unlike conventional Fabry–Pérot or multilayered designs, which require distinct thicknesses and costly nanofabrication to achieve multiple colors, our approach demonstrates that diverse spectral responses can be encoded within a uniform-thickness cavity through localized modulation of nanoporous morphology.This advancement offers a scalable, lithography-free route to multicolor rendering, validated on centimeter-scale substrates. The uniform cavity AAO structures are achieved via complete anodization of an aluminum thin film, and local modulation of AAO porosity works as a versatile design method. The demonstrated artwork-like multicolor images highlight both the scientific precision and expressive versatility of the method. Because AAO anodization is already a widely used process for large aluminum components, the approach can be extended seamlessly to much larger surfaces. This compatibility underscores strong potential for industrial translation, where large-area, durable, and robust color platforms are required. The insight establishes index modulation as a general design lever in nanophotonics, shifting the field from geometry constraints to optics based on morphology and extending beyond coloration to metasurfaces, flat optics, anti-counterfeiting, and integrated optoelectronics. |
In industrial fields including art, architecture, and fashion, color implementation has mainly relied on material-based technologies. Electronic devices also employ dye- and pigment-based color resists in color filter systems including displays and imaging sensors. However, its inherent dependence on material properties imposes several limitations. One major limitation is its poor environmental stability, as it remains susceptible to ultraviolet radiation, thermal stress, and chemical degradation.17 The size of pigment particles is an additional obstacle for obtaining high quality of color. Submicron particles increase scattering and consequently reduce saturation, whereas conventional larger pigments (∼10 μm) decrease pixel density and resolution.18
In contrast, structure-based colors provide material-independent, high-resolution color control via light–matter interaction on subwavelength scales, with remarkable stability and reproducibility. Although nanophotonic phenomena such as surface plasmons, Fabry–Perot (FP) interference and photonic bandgaps, are well organized in classical theory, their practical implementation remains a significant challenge. The fabrication technology of nanostructures has seen remarkable advancements since the early 2000s, expanding their applicable domains. Nevertheless, most of the structural colors encounter constraints regarding scalability and manufacturing cost. Generally employed nanopatterning methods such as electron-beam lithography or focused ion beam processing are costly and time-consuming11,12 for mass production. For these reasons, most reported studies have demonstrated various hues and intricate patterns in the microscale (∼μm2), or are often limited to single-chroma reproduction when scaled up to the centimeter-scale.19–21
In this study, we suggest a novel approach to structural coloration by incorporating a spatially modulated anodic aluminum oxide (AAO)22 layer as the insulator in a metal–insulator–metal (MIM) structure. The MIM structure shows superior color selectivity based on FP interferences, and consists of stacks of thin films, quite simple compared to other structural colors. Since the resonance wavelength is dependent on the cavity thickness,23,24 different thicknesses are required for RGB implementation, and multilayer fabrication and additional masking steps are required.25,26 Unlike thickness-dependent FP tuning, our method leverages porosity-driven refractive index engineering to achieve color selectivity in a constant-thickness cavity, establishing a new methodology in structural coloration. This enables multiple resonance wavelengths to be achieved within a constant thickness MIM cavity, addressing the conventional limitation of thickness-dependent tuning. Importantly, lithography-based multicolor implementation usually demands multiple masks,25,26 overlay-critical steps,27 photoresist coat/bake/develop cycles,28 and dry/wet etching,29 particularly when RGB is achieved by thickness-split cavities.23,24 By contrast, our approach achieves nanoscale patterning through self-organized AAO in a single, low-temperature wet step without the need for a photoresist or etching. Spatial selectivity is introduced lithography-free by selective anodization (using simple local masking during anodization) and a single shadow-mask deposition for artwork patterns. Combined with the constant-thickness cavity design, these factors reduce process complexity and reliance on capital lithography tools, providing a cost-effective route that is compatible with established industrial anodization.22,30–33 By employing anodization, a simple and industrially common process, we generate vivid multicolor patterns without lithography. The proposed fabrication flow with a thin-film type of aluminum (Al) and spatial growth of AAO could realize the artwork-like and scalable multicolor patterns in a single substrate. As anodization is already being practiced on large Al surfaces (even aircraft wings),30,33 our strategy can be seamlessly scaled from centimeter demonstrations to wafer- or industrial-scale devices.
The dimensions of the anodic alumina layer, including interpore distance and pore diameter, are considerably smaller than the operating wavelengths in the visible regime. Under such subwavelength conditions, the AAO cannot be treated by simple ray optics; instead, the porous structure can be regarded as an effective homogeneous medium from the electromagnetic perspective. In this approach, light propagation is described by an averaged refractive index that depends on the porosity of the layer. Eqn (1) therefore represents the effective refractive index (neff) of the porous AAO, calculated by applying an effective medium approximation that accounts for the volume fractions of alumina and air. As the porosity increases, neff decreases toward the refractive index of air, while lower porosity results in a higher neff closer to bulk alumina. This effective index treatment provides a valid approximation for modeling the optical response of the AAO cavity and is commonly employed in porous photonic films. This optical design method relies on modulating the neff of the AAO layer to achieve various resonance wavelengths. The values of neff refer to the volume-averaged refractive index of the nanoporous Al2O3 cavity layer, which is tunable through control of the pore geometry. The neff is calculated based on the porosity (φ) of a hexagonally arranged pore structure as follows,
![]() | (1) |
The cavity consists of an AAO layer with a nanoporous, where neff is tunable by porosity control as follows,
![]() | (2) |
The resonant wavelength is determined by the cavity thickness, reflection-induced phase shifts, and the travelling phase of light in the cavity, which is determined by neff. As shown in Fig. 1d, the resonance wavelengths of the primary colors, the red (R), green (G), and blue (B), are modulated through the control of neff under a constant cavity thickness condition. Fig. 1d shows that the simulated transmittance spectra of the RGB meta-MIM structures exhibit resonance peaks at the designed wavelengths of 700 nm (R), 510 nm (G), and 462 nm (B). These resonant modes are caused by constructive interference within the cavity layer of constant thickness and demonstrate high spectral selectivity. The intensity of each peak indicates the efficiency of light transmission through the nanoporous cavity under resonant conditions. Resonance wavelengths of 700 nm, 510 nm, and 462 nm are achieved within the 250 nm cavity, corresponding to neff = 1.26 (R), 1.73 (G), and 1.56 (B), respectively, with porosity (φ) of 0.70 (R), 0.08 (G), and 0.32 (B).
For the red chroma, the constructive interference mode corresponds to the first-order resonance mode, whereas the green and blue chroma originate from the second-order resonance mode. Simulated electric field profiles for the RGB structures are shown in Fig. 1e. The red device exhibits four periodic units, while the green and blue devices show two periodic units each. The black dashed lines indicate the positions of the AAO holes. The red device exhibits a single antinode, which is indicative of a fundamental (first-order) mode, while two antinodes are observed in the green and blue structures, corresponding to second-order resonance modes. These field profiles are in excellent agreement with the design model presented in eqn (2). As illustrated in Fig. 1f, the Ag–AAO cavity interface introduces wavelength-dependent reflection phases, and the corresponding calculated phase spectra are provided in Fig. S3. The combined reflection phases of Ag–AAO (Δφtop + Δφbottom) and propagation phase (2neffdk0) within the AAO cavity satisfy a total phase of 2mπ (R: m = 0, G and B: m = 1), depending on the effective optical path determined by the porosity and thickness. In this structure, the red corresponds to a first order mode, whereas the green and blue represent second order mode. The total phase difference, including both propagation and reflection components, satisfies the resonance condition of 2mπ for each color. This enables spectrally selective resonance within the same physical cavity thickness (250 nm), by tuning the neff via porosity modulation.
Fig. 2a depicts the transmission spectra at various porosities. The red line corresponds to a first-order resonance mode, while the other colors represent a second-order resonance mode. As the porosity increases, the resonance wavelength shifts toward the blue. The estimated neff values align well with the theoretical values derived from eqn (2).
The color palette was calculated from a parametric sweep of the nanoporous cavity design, in which the interpore distance (Dint: 50–400 nm) and pore diameter (Dp: 20–400 nm) are varied independently, as shown in Fig. 2b. This two-dimensional design space allows continuous modulation of neff of the AAO cavity. This allows wide range tunability for the resulting structural colors while maintaining the physical cavity thickness unchanged. The light brown area in the palette represents the physically unattained configurations where Dp exceeds Dint, indicating a pore-dominant regime with neff approaching to that of air.
Fig. 2c shows the simulated spectral outputs of the cavity structures in the CIE 1931 color coordinate system, providing an intuitive visualization of the achievable color gamut. Each plotted point corresponds to a distinct (Dint, Dp) combination and demonstrates that a single-cavity configuration can support a wide range of vivid, high-purity colors. This highlights the ability of the proposed design to deliver full-color images through precise control of nanostructural parameters.
For the selective control of a single resonant wavelength within a cavity on the subwavelength-scale, the use of low-order resonant modes is essential. As a result, the cavity length must be confined to less than 300 nm, which confines the design range for photonic structure. The effective refractive index is tunable in the range of 1.1 to 1.8. In our structure, the blue–green resonances originate from the second-order mode, which is relatively insensitive to reflection-phase variations at the Ag/AAO interfaces. By contrast, the yellow–red region corresponds to the first-order resonance, which is more strongly influenced by the wavelength-dependent reflection phases of Ag. When eqn (2) is applied to the yellow spectral region (≈580 nm), the propagation phase must contribute ∼1.6π (for m = 0) or ∼3.6π (for m = 1) in order to satisfy the total phase condition. This corresponds to neff of approximately 0.92 or 2.1. Such values lie well outside the physically attainable range of porous AAO (1.1–1.8), thereby preventing the formation of a resonance in this region. This quantitative analysis clarifies why the yellow channel does not emerge in the actual spectra, whereas the RGB resonances remain accessible within the achievable design space. Despite these limitations, it is still possible to achieve distinct resonances at the primary RGB wavelengths. This is particularly significant for color-selective imaging applications, where the excitation of red, green, and blue resonances is the foundational requirement for color reproduction.
To enable neff tuning, nanoporous patterning is introduced using a self-ordered AAO process. Prior to anodization, nail polish masking is applied to separate the working areas as a drawing-like approach, allowing the formation of several different nanostructures on a single substrate. Anodization is then obtained by applying a controlled voltage in an acidic electrolyte, forming a vertically aligned Al2O3 nanopore array with specific dimensions of Dint and Dp. The dimension of Dint is directly proportional to the applied voltage, while that of Dp can be independently adjusted through a pore-widening process.31 In regions coated with nail polish, the electric field is excluded and anodization does not occur, enabling spatial pattern variation. After anodization, the specimen is rinsed with acetone and IPA. To create multiple colors (‘N’ configurations) on the same substrate, the above steps are repeated N times with different pore-widening durations, allowing selective modulation of Dp under fixed Dint conditions.
In addition, to achieve gradual coloration, spatial modulation of the pore diameter was realized by controlling the pore widening duration in a region-dependent manner. Without a repeated masking process, this can be accomplished by progressively immersing different regions of the sample in phosphoric acid, thereby inducing spatial variation in the etching time. After pore engineering, the MIM structure is completed via the deposition of a top Ag reflector (20 nm) and a WO3 capping layer (70 nm) to improve the optical outcoupling as illustrated in Fig. S2a. At this stage, shadow mask is used for artwork or specific patterning.
Fig. 4 illustrates the experimental results of the fabricated meta-MIM structures, including measured transmittance spectra, photographs, and field emission scanning electron microscope (FE-SEM) images of the uniform-cavity meta-MIMs. The single chroma of R, G, and B were fabricated in a 2 cm × 2 cm area. As shown in Fig. 4b, the transmittance spectra and corresponding photographic images of the R, G, and B structures reveal resonance wavelengths at 700 nm (R), 521 nm (G), and 441 nm (B). The peak positions of the green and blue devices have shifted slightly compared to the designed values. The peak intensities were measured to be 46.6% (R), 31.04% (G), and 33.33% (B), representing a 30–50% reduction compared to the simulation results.
This deviation originates from two main sources. Firstly, the optical simulations were based on well-ordered AAO nanostructures. The systematic regular patterns, typically achieved through a two-step anodization process31 require thick Al media. In contrast, the suggested devices were fabricated using a single-step anodization with a thin Al film, leading to lower pore ordering and irregular morphology, as shown in Fig. 4c and d. Moreover, incomplete pore penetration was observed in some regions, introducing additional structural irregularities. This structural disorder reduces the quality of optical resonance.
Second, surface roughness and thickness variations at the top surface of the porous AAO layer can lead to non-uniform deposition of the top Ag and WO3 layers. These irregularities distort the FP resonance condition by disrupting phase matching within the cavity. In particular, since the resonant phase shift is highly sensitive to the reflective phase of Ag, even minor roughness can induce phase errors, resulting in spectral shifts and transmittance loss. Overall, the measured red-shift and reduced transmittance are attributed to these optical non-idealities of the fabricated structures. Nevertheless, these results validate the proposed design approach and suggest that precise color reproduction can be further improved through process optimization and thin-film quality control.
As shown in Fig. S4, the FDTD optical simulation results based on SEM-derived structures exhibit better agreement with the experimental data than those based on idealized geometries. This improved correspondence arises from the incorporation of actual morphological features observed in SEM images, such as irregular pore shapes and incomplete hole penetration. To more accurately reflect the real morphology seen in Fig. 4e—where certain nanopores do not fully penetrate through to the bottom Ag layer—a modified FDTD model was constructed by introducing randomly distributed non-penetrating holes with residual thicknesses of approximately 30–50 nm. This modification enabled a more realistic optical response by accounting for the imperfect pore formation commonly found in the fabricated AAO.
In particular, for the blue device, the simulated resonance wavelength appears at 454 nm, while the experimental value is 432 nm—showing a blue shift of approximately 22 nm, yet preserving the overall spectral shape. The SEM-based simulated peak transmittance was 43.73%, while the experimental value was 33.36%, corresponding to a reduction of 23.7% relative to the simulation results. This discrepancy is primarily attributed to imperfect surface flatness of the AAO layer and the deposited films, which introduce deviations from ideal FP cavity conditions. This interpretation is further supported by atomic force microscopy (AFM) images in Fig. S5, which reveal that the AAO-based structure exhibits significantly higher surface roughness than the reference device, with root mean square (RMS) roughness values of 8.557 nm and 2.516 nm, respectively. Additionally, the broader FWHM observed in the experimental spectrum is attributed to thickness non-uniformity and morphological imperfections in the AAO structure, both of which degrade spectral confinement within the resonance cavity.
A critical aspect of the proposed fabrication procedure is that the Al medium utilized to create the AAO layer must be deposited as a continuous single film throughout the entire substrate. This approach provides sufficient electrical continuity, helping to maintain a stable electric field during anodization, as explained in Fig. S6. If an artwork-like or free-styled pattern is pre-defined during Al deposition prior to anodization, the zero potential areas due to the electrical discontinuity are not available for oxidation. Because of the thin film thickness, the Al media undergo fully processed oxidation and convert to insulating media, thus stopping the electric channel. Thin film Al and fully anodization realize a uniform thickness of the cavity. Furthermore, since conductor surfaces are fundamentally equipotential, the direction and strength of the local electric field might become skewed near the borders of patterned patches, inducing lateral growths of the pores.
Fig. 5 illustrates the versatility of AAO-based structural coloration through a series of spatially patterned demonstrations. Within a single substrate, we reproduced a replica of Nadia aux cheveux lisses by Henri Matisse with gradual-color and campus nameplates (KNU) with multi-color, emphasizing the convergence of scientific precision and artistic expression. In Fig. 5a, the letters “K”, “N”, and “U” are displayed in different colors on a single substrate. These colors were realized by spatially varying the AAO pattern in each region within a uniform cavity. Fig. 5b confirms that the same fabrication strategy can be applied to flexible substrates, maintaining both color integrity and mechanical stability during bending. Fig. 5c presents the original line drawing Nadia aux cheveux lisses by Henri Matisse, which served as the design motif. The corresponding shadow mask, shown in Fig. 5d, was used to reproduce the artwork using a single-step deposition process. This avoided complex lithographic alignment and enabled high-fidelity patterning over a large area.
Finally, Fig. 5e demonstrates gradual color variation within a single image, achieved by continuously tuning the AAO pore diameter. This result illustrates the ability of the method to spatially pattern both discrete and continuous color information, opening possibilities for scalable fabrication of multifunctional and visually expressive nanophotonic elements. Notably, the entire image was patterned using a single shadow mask, and color separation was accomplished through selective deposition of the top reflective layer. This eliminates the need for complex mask alignments or multiple masking steps, thereby simplifying the fabrication.
The proposed meta-MIM modulates neff within the AAO cavity of constant thickness, enabling precise optical resonance tuning. This is obtained through the geometric control of a nanoporous AAO layer, where the Dint and Dp determine the neff. The resonance conditions defined in Eqn (2) enable resonance wavelength control on large-area substrates, relying primarily on this geometric modulation rather than on cavity thickness or material. The proposed optical design maintains the benefits of FP, as it can be adjusted by the average porosity ratio rather than accurate periodicity or size control in the AAO pattern. Simulations confirmed RGB resonances could be tuned by neff at constant cavity thickness. Fabricated devices exhibited visible colors but with slight spectral shifts and lowered intensity due to roughness and pore irregularities. This validates the conceptual advance of decoupling resonance from geometry to porosity-driven index control.
Specifically, surface roughness and pore irregularities in the single-step anodized AAO layer hinder uniform deposition of the upper Ag and WO3 layers. These imperfections introduce phase mismatches in the cavity, resulting in spectral deviations and broadened transmittance profiles. To address these issues, future work could explore the use of ultrathin buffer layers such as atomic layer deposition (ALD) to improve the planarity of the AAO surface without compromising porosity. Additionally, employing oblique-angle metal evaporation or implementing mild post-anodization surface etching may help achieve smoother top interfaces, thereby enhancing FP resonance fidelity. These refinements can further improve color purity and transmittance efficiency, expanding the practical applicability of meta-MIM systems.
Nevertheless, the close alignment between measured and simulated spectra confirms the robustness of the design strategy. In addition, the meta-MIM exhibits remarkable scalability and spatial multiplexing capabilities. For large area applications, recent advances in printing-based structural coloration including nanoimprint lithography (NIL), inkjet printing, and roll-to-roll (R2R) processes, have enabled centimeter-scale multicolor rendering with high throughput.39–45 But these approaches typically rely on costly mold fabrication, residual layer removal, and overlay critical alignment. Inkjet printing provides mask-free, digital patterning with design flexibility, yet its resolution remains limited to the micrometer scale and uniformity is challenged by droplet variability. In contrast, our AAO-based approach realizes color selectivity in a constant-thickness FP cavity through porosity-driven effective refractive index modulation, thereby eliminating thickness splitting and high-resolution lithography. Because the nanoporous AAO is formed by self-ordering in a single low temperature wet step, spatial selectivity can be realized via selective anodization and a single shadow mask deposition. This combination offers process simplicity, compatibility with photolithography for more complex designs, and industrial scalability, as anodization is already practiced over meter-scale aluminum components. While the optical figure-of-merit (intensity/FWHM) of our devices remains comparable to previously reported dielectric46–48 or plasmonic filters,49–51 the unique advantage of our method lies in its scalability and versatility, enabling multifunctional full color designs such as artwork reproduction and flexible integration. This constitutes a distinct performance axis beyond spectral purity alone.
Localized masking and selective pore expansion can be used to pattern distinct nanoporous geometries on a single substrate, supporting spatially resolved multicolor rendering at uniform cavity thickness. The artwork-like nature of these demonstrations emphasizes expressive versatility, suggesting applications in anti-counterfeiting, aesthetic photonics, and wearable displays. Spatial control of anodization provides lithography-free patterning that is inherently scalable. Moreover, because anodization is compatible with large-area industrial practice, the method offers strong potential for translation from centimeter-scale demonstrations to wafer-level substrates and industrial components.
| This journal is © The Royal Society of Chemistry 2025 |