Open Access Article
Bolim
You‡
a,
Jeechan
Yoon‡
ae,
Yuna
Kim
a,
Mino
Yang
b,
Jina
Bak
a,
Jihyang
Park
a,
Un Jeong
Kim
*d,
Myung Gwan
Hahm
*ac and
Moonsang
Lee
*a
aDepartment of Materials Science and Engineering, Inha University, 100 Inha-ro, Michuhol-gu, Incheon 22212, Republic of Korea. E-mail: mghahm@inha.ac.kr; mslee@inha.ac.kr
bKorea Basic Science Institute Seoul, 6-7, Goryeodae-ro 22-gil, Seongbuk-gu, Seoul 02841, Republic of Korea
cInstitute for Bio-Medical and Translational Health Care, Inha University Hospital, 27 Inhang-ro, Jung-gu, Incheon 22332, Republic of Korea
dDepartment of Physics, Dongguk University, Seoul 04620, Republic of Korea. E-mail: ujjanekim@dongguk.edu
eWONIK IPS CO., LTD, 75, Jinwisandan-ro, Jinwi-myeon, Pyeongtaek-si, Gyeonggi-do, Republic of Korea
First published on 12th April 2024
Neuromorphic electronics are gaining significant interest as components of next-generation computing systems. However, it is difficult to develop flexible neuromorphic electronics for implementation in various edge applications such as bio-implantable electronics and neuroprosthetics. In this study, we present a reconfigurable 2D tellurene (Te) artificial synaptic transistor on a flexible substrate for neuromorphic edge computing. Single-crystalline 2D Te flexible synaptic transistors exhibit potentiation and depression modulated by gate pulses with an extremely low power consumption of 9 fJ, 93 effective multilevel states, excellent linearity and symmetry, and an accuracy of 93% in recognizing the Modified National Institute of Standards and Technology (MNIST) patterns. Furthermore, it was observed to be a flexible synaptic transistor with outstanding gate tunability and endurance characteristics, even under a 2% curvature in both the concave and convex states. We believe a robust 2D Te flexible artificial synapse will effectively function as a building block for wearable neuromorphic edge computing applications.
Furthermore, a high demand exists for neuromorphic electronics with flexible functionality for implementation in various edge applications such as wearable,15,16 bio-implantable,17,18 and soft electronics,19 interactive robotics,20 and neuroprosthetics.21 Flexible electronics with neuromorphic platforms present considerable potential in connecting edge devices with cloud computing to provide intelligence and AI services in real time, leading to a hyperconnected era. Flexible electronic devices with low power consumption and high performance are crucial for realizing edge devices, and flexible synaptic electronics are suitable since they exhibit these characteristics.22,23 Various materials such as metal oxides,24,25 quantum dots,9,26 organic materials,27,28 perovskites,29,30 nanowires,31,32 and two-dimensional (2D) nanomaterials33–35 have been used to satisfy these requirements. In particular, 2D nanomaterials are highly promising owing to their unique characteristics, such as excellent flexibility, thermal and mechanical stability, strong electrostatic tunability, low power consumption, monolithic integration, and high scalability.36–39 Among them, 2D Te presents excellent mechanical flexibility, environmental stability, and optoelectronic tunability, along with high carrier mobility, which can provide a breakthrough for implementing flexible electronics for neuromorphic edge computing.40–44 Previous studies have reported 2D Te synaptic devices with ultra-low power consumption, excellent synaptic plasticity, and environmental stability, demonstrating the potential of 2D Te for implementation in synaptic devices.45
In this study, we present a 2D Te flexible artificial synaptic transistor for bio-inspired wearable neuromorphic edge computing. Flexible artificial Te synapses exhibit an ultralow energy consumption of 9 fJ, 93 effective multilevel states, and excellent short- and long-term plasticity with good linearity and symmetry even under a 2% curvature in both the concave and convex shapes. The simulation of the Modified National Institute of Standards and Technology (MNIST) pattern recognition accuracy presents a high pattern recognition accuracy of 93%, demonstrating excellent biological synaptic imitation. Particularly, stable synaptic characteristics without significant degradation under compressive and tensile stress demonstrate the excellent potential of neuromorphic edge computing architectures in wearable applications. We believe that this study provides a strong foundation for a flexible, artificial synapse-based neuromorphic edge computing architecture.
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1
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2 ratio. After 3 days, 0.1 mL of the thinned solution and 0.9 mL of ethanol were placed in a centrifuge and spun at 1000 rpm for 5 min. Then, the ethanol was removed entirely, leaving only Te flakes, and 0.9 mL of DI water was added. Drop-casting was performed on the substrate using this solution, followed by cleaning with acetone, IPA, and DI water to obtain an extremely thin 2D Te material.
000 MNIST images with 28 × 28 pixels, comprising handwritten digits from 0 to 9, were trained using the backpropagation algorithm. Subsequently, the MNIST pattern recognition test was performed on 10
000 images.
0] direction in the transmission electron microscopy (TEM) mode using an aperture with a radius of 30 μm. The high-angle annular dark-field (HAADF) image in Fig. 1(b), captured in the scanning transmission electron microscopy (STEM) mode, demonstrates that the synthesized Te flakes form a perfect 2D atomic structure at the atomic level. It can be observed that the atomic structure in this image is three-fold symmetric with a helical chain along 〈0001〉, and the interplanar distances of the (1
10) and (0001) planes were ∼2 and 6 Å.46 Raman spectroscopy was conducted to elucidate the atomic vibrational mode of the synthesized atomic-layered Te, as shown in Fig. 1(c). The Raman spectrum of the Te flakes illustrates four vibrational modes located at 91.8, 103.4, 120.3, and 139.7 cm−1 corresponding to the E1-TO, E1-LO, A1, and E2 peaks.40 The Raman mapping images of the 2D Te flakes exhibit uniform Raman spectral distribution (Fig. S2, ESI†). This indicates that the 2D Te flakes present a uniform crystalline quality in all the regions. X-ray photoelectron spectroscopy (XPS) was performed to analyze the chemical composition of the Te nanoflakes as shown in Fig. 1(d). The XPS energy levels of Te 3d3/2 and 3d5/2 are located at 582.6 and 572.1 eV, which are attributed to the spin–orbit doublets of the Te–Te bond, respectively. The small peak is attributed to the Te–O bond, indicating a slight oxidation in the hydrothermal process.47Fig. 1(e) shows the height profile of the Te nanosheet with a thickness of 16 nm, which is obtained using atomic force microscopy (AFM). Kelvin probe force microscopy (KPFM) analysis was then performed to confirm the charge distribution on the surface of the Te nanoflake, as shown in Fig. S3 (ESI†). The difference in the surface potential distribution between Te and p-Si was estimated to be ∼0.12 V, indicating that the Te nanoflakes present a work function of ∼5.06 eV, which is consistent with the literature.48
The electrical characteristics of the h-BN/Te device were studied to determine its feasibility as an artificial synapse. A flexible h-BN/Te top-gate device was fabricated on a polyethylene terephthalate (PET) substrate, as shown in Fig. 2(a). Considering the variation in electrical characteristics based on the crystal orientation of 2D Te, a device channel with a length of 3 μm and a 3 μm width between the source and drain was constructed along the [0001] direction through the conventional photolithography technique (Fig. S4, ESI†).40 A charge-trapping layer must be formed to facilitate charge-trapping or de-trapping.49 We made the channel conductivity adjustable by applying O2 plasma treatment to h-BN (Fig. S5, ESI†). The Raman spectra and Raman mapping images of the h-BN transferred onto Te demonstrate that h-BN uniformly encapsulated the entire Te nanoflake, indicating the formation of a charge-trapping layer in all regions of the 2D Te flake (Fig. S6, ESI†). Fig. 2(b) illustrates the electronic transfer characteristics of the h-BN/Te device at VDS = 0.01 V. The transfer curve exhibits a threshold voltage (VTH) of 7.23 V with p-type conductivity. Furthermore, the h-BN/Te field-effect transistor (FET) showed a field-effect mobility of 56.2 cm2 V−1 s−1, along with a subthreshold swing of 2.06 V per decade. The current on/off ratio within a 20 V bias is 3.6 × 102. These results demonstrate that the h-BN/Te top-gate device was effectively fabricated. The output characteristics of the FET exhibit distinct symmetric and linear behaviors. This indicates the successful formation of Ohmic contacts within the source and drain electrodes, as shown in Fig. 2(c). Notably, anticlockwise hysteresis characteristics were observed in Fig. 2(d), indicating that the operating mechanism is charge-trapping or de-trapping.50 The hysteresis window was broadened with the increase in ΔVGS. These gate-controlled electronic transfer characteristics verify the existence of programmable multilevel conductance states in the h-BN/Te FET. We exposed the h-BN/Te device to ambient conditions for 3 weeks to demonstrate its environmental stability. The transfer characteristics of the h-BN/Te device exhibited negligible hysteresis and current level changes for 3 weeks under ambient conditions, as shown in Fig. 2(e). In addition, a slight variation in VTH was observed in the write and erase operation modes over 1000 cycles, indicating excellent reliability (Fig. 2(f)). These results demonstrate that the h-BN/Te top-gate transistor is suitable for wearable synaptic devices.
Biological synapses are microscopic gaps between the pre- and postsynaptic terminals.51,52 A presynaptic neuron generates an action potential when an input spike exceeding the threshold is applied. Subsequently, neurotransmitters are released from the presynaptic terminals and engage with receptors on the dendrites of the postsynaptic terminals. Owing to this interaction, the synapses shape the biological memory and behaviors of human beings.53 We reconfigured the gate and drain electrodes of the 2D Te FET as the presynaptic and postsynaptic neurons, respectively, to replicate these interactions. To confirm the short-term synaptic plasticity of the wearable artificial synaptic transistors, we explored their excitatory and inhibitory postsynaptic current (EPSC and IPSC) characteristics, as shown in Fig. 3(a)–(f) where different pulse amplitudes and time durations were applied to the gate-generated PSCs in the artificial synapses.
Fig. 3(a) illustrates the EPSC characteristics of the flexible 2D Te artificial synaptic transistors as a function of different gate voltages (VGS) under a constant drain read voltage of 0.01 V and pulse width of 100 ms. The increase in the gate voltage amplitudes from 3 to 7 V increased the ΔPSC from 65 to 217 nA. Furthermore, the increase in the spiking pulse width increased the EPSCs at a fixed pulse magnitude of 3 V and read voltage of 0.01 V, as shown in Fig. 3(b). Additionally, an increased VDS resulted in enhanced EPSCs, as shown in Fig. 3(c). Fig. 3(d) and (e) show the IPSC contours for an identical platform. They exhibited a trend similar to that of the EPSC characteristics, except for the opposite negative pulse polarity. These results demonstrate that the electrical modulations of the pre- and postsynaptic terminals regulate the short-term synaptic plasticity of the flexible 2D Te artificial synaptic transistors, indicating excellent replication of biological networks. We analyzed the paired-pulse facilitation (PPF) of the flexible 2D Te artificial templates to obtain a deeper insight into their short-term synaptic plasticity characteristics, as shown in Fig. 3(f). PPF is a form of short-term synaptic plasticity triggered by presynaptic spikes with pulse interval times (Δt) and defined by A2 over A1.54,55 Here, A1 and A2 represent the peaks of the first and second PSC spikes, respectively, as shown in the inset of Fig. 3(f). The strength of PPF in the artificial platform steadily weakened with the increase in Δt. The short-term plasticity strength of the flexible 2D Te artificial synaptic transistors clearly belongs to the following double exponential decay equation:56
![]() | (1) |
| Econsumption = Vread × Ipeak × tpulse, | (2) |
We analyzed the long-term potentiation (LTP) and depression (LTD) characteristics of flexible 2D Te artificial synaptic transistors under various electrical presynaptic triggers to elucidate their long-term synaptic plasticity and reconfigurable capacity. Fig. 4 depicts five different LTP/LTD patterns of the artificial synaptic transistor under 100 consecutive electrical potentiation and depression-spiking modulations. One hundred constant single pulses with an amplitude of 4 V, a pulse width of 50 ms, and an impulse interval time of 70 ms were applied for both potentiation and depression, as shown in Fig. 4(a). They demonstrate robust write and erase operations for learning and memory behaviors in the flexible artificial synapses. This presented an abrupt increase in the conductance for both the LTP and LTD. The corresponding potentiation impulse and decreased gate spiking magnitude from −4 to −1 V in the depression array resulted in a moderately decreased slope in the LTD, as shown in Fig. 4(b). Fig. 4(c) illustrates the ascending stepwise gate impulse magnitude arrangement from 1 to 4 V for the potentiation and the depression at a fixed negative spiking progression of −1 V. A more moderate increment in conductance in the LTP sequence was observed when compared to that in Fig. 4(b). A stepwise presynaptic electrical spiking array from 1 to 4 V in both the potentiation and depression arrangements improved the symmetry of the LTP/LTD curve, as shown in Fig. 4(d). A reduced gate spiking magnitude of −0.1 V with a spiking step of 40 mV at the starting point of the depression arrangement and the corresponding potentiation bias from Fig. 4(e) shaped a more balanced erasing feature in the depression stage. The gate tunability of the learning feature governs the figure-of-merit of the artificial synaptic devices, such as multilevel states, the dynamic range, symmetry, and linearity.62 The high multilevel states improve the training capability and robustness of the device. The dynamic range, which is the ratio between the maximum conductance (Gmax) and minimum conductance (Gmin), is crucial in terms of the power consumption and mapping capability.63 The symmetry and linearity of the LTP/LTD curve can improve the recognition accuracy of the artificial neural network system. The linearity and symmetry of the LTD/LTD for the flexible 2D Te artificial synaptic transistor were estimated as follows:64
| Gp = B(1 − e−P/Ap) + Gmin, | (3) |
| Gd = −B(1 − e(P−Pmax)/Ad) + Gmin, | (4) |
![]() | (5) |
![]() | (6) |
Electrical stability under mechanical modulation is highly promising for flexible electronics such as wearable edge computing, soft robotics, and neuroprosthetics. To elucidate the mechanical stability and flexibility of the flexible 2D Te artificial template, we analyzed the LTP and LTD stabilities of the 2D Te artificial synaptic transistors under different bending strains, as shown in Fig. 5. Fig. 5(a) shows a photograph of a flexible 2D Te FET mounted on a PET substrate with a bending force. Fig. 5(b) shows the endurance characteristics in the flat, convex, and concave bending states. The bending strain was calculated as ε = t/ρ, where t denotes the thickness of the substrate and ρ denotes the bending radius (Fig. S7, ESI†).65 The trajectory of the LTP/LTD sequence was achieved by applying 2000 sequential electrical pulses for VGS, from 1 to 4 V (with a ΔV of 30 mV) for potentiation and from 0.1 to 4.1 V (with a ΔV of 40 mV) for depression, along with a VDS of 0.01 V. It can be observed that the flexible 2D Te artificial synaptic transistors exhibit excellent mechanical stability and reconfigurability via gate tunability, regardless of the bending status on the devices, demonstrating their potential for future applications (Table S3, ESI†). Notably, artificial synapses with convex and concave bending exhibited 100 and 79 effective states, respectively. The effective state in the flat state was 93. Furthermore, the flexible artificial synaptic transistor with concave bending exhibited a much lower conductance level over the entire measurement range when compared to other synaptic devices. These characteristics are attributed to the generation of the piezoelectric field and variation in the surface contact area of O2 or H2O molecules. The piezoelectric effect occurs when strain is applied to the lattice of Te, which has a trigonal crystal lattice structure. This strain causes a deformation that eliminates the inversion symmetry of the Te crystal lattice, leading to the emergence of ion charge polarization.66 In this case, according to the convenience of piezoelectric theory, the piezoelectric polarization charges are regarded as surface charges on the bulk piezoelectric material.67 When a negative piezoelectric polarization charge is induced in a p-FET, it causes the majority carriers, which are holes, to accumulate at the interface, resulting in a reduction of the Schottky barrier height (SBH). Conversely, the induction of a positive piezoelectric polarization charge repels holes from the interface, leading to an increase in the SBH.68 In convex bending, a negative piezoelectric polarization charge is induced on the source–Te interface and a positive charge on the drain–Te interface. This leads to a decrease in the SBH at the source side and an increase at the drain side, facilitating the flow of more holes and improving FET conductance. Conversely, in concave bending, a positive piezoelectric polarization charge is induced on the source–Te interface and a negative charge on the drain–Te interface. This results in an increased SBH at the source side and a decreased SBH at the drain side interface, causing a reduction in hole flow compared to the flat state and resulting in reduced performance. Furthermore, the crystallographic orientation of the Te lattice can govern the direction of the piezoelectric polarization charge.69,70 This nature is currently under study. Another reason for conductance changes due to bending is changes in the surface contact area of O2 or H2O molecules, which can change the amount of charge carrier trapping/detrapping, leading to changes in conductance values.71,72 Based on the results of the 10 cycles LTP/LTD curve, we implemented a backpropagation algorithm to confirm the learning and recognition characteristics of artificial neural network (ANN) simulation. The network structure is a simple model, as shown in Fig. 5(c). It is a two-layer perceptron neural network with 784 input neurons, with 300 neurons in the hidden layers and 10 neurons in the output layers. We used handwritten digits of 28 × 28 pixels based on the MNIST dataset. The pattern recognition accuracy was indicated by 40 training epochs, and Fig. 5(d) shows the simulation results of the flexible 2D Te synaptic transistor with different strains. In the case of convex bending, the artificial 2D Te synaptic transistor immediately achieved an accuracy of 90% in the first training epoch and subsequently achieved a high recognition rate of 94%. The flexible 2D Te artificial platform with concave bending exhibited an accuracy of approximately 88%, which is slightly lower than the accuracy of 93% in the flat state but still considered a comparable or superior level compared to those of previous studies.45,73 In conclusion, the flexible 2D Te artificial synaptic transistor presents considerable potential in wearable neuromorphic edge computing devices requiring outstanding mechanical stability.
Footnotes |
| † Electronic supplementary information (ESI) available: Schematics of solvent-assisted thinning and drop casting processes, OM and Raman mapping images of 2D Te, surface potential and work function of 2D Te on p-type Si, schematics and OM images of the fabrication method for the flexible 2D Te transistor, data of the comparison before and after O2 plasma treatment on h-BN, schematics of the concave and convex bending models, table summarizing the gate tunability performance of the 2D Te synaptic transistor, performance comparison of previously reported 2D material-based synaptic devices, and performance summary table of convex and concave bending of a 2D tellurium flexible FET (PDF). See DOI: https://doi.org/10.1039/d4tc00530a |
| ‡ These authors contributed equally to this paper. |
| This journal is © The Royal Society of Chemistry 2024 |