Skip to main content
Science Advances logoLink to Science Advances
. 2024 Apr 17;10(16):eadn4524. doi: 10.1126/sciadv.adn4524

Ultralow-power optoelectronic synaptic transistors based on polyzwitterion dielectrics for in-sensor reservoir computing

Xiaosong Wu 1,2,3,, Shuhui Shi 4,, Baoshuai Liang 1,2,3, Yu Dong 1,2,4, Rumeng Yang 1,2,3, Ruiduan Ji 1,2,3, Zhongrui Wang 4,*, Weiguo Huang 1,2,3,*
PMCID: PMC11023521  PMID: 38630830

Abstract

Bio-inspired transistor synapses use solid electrolytes to achieve low-power operation and rich synaptic behaviors via ion diffusion and trapping. While these neuromorphic devices hold great promise, they still suffer from challenges such as high leakage currents and power consumption, electrolysis risk, and irreversible conductance changes due to long-range ion migrations and permanent ion trapping. In addition, their response to light is generally limited because of “exciton-polaron quenching”, which restricts their potential in in-sensor neuromorphic visions. To address these issues, we propose replacing solid electrolytes with polyzwitterions, where the cation and anion are covalently concatenated via a flexible alkyl chain, thus preventing long-range ion migrations while inducing good photoresponses to the transistors via interfacial charge trapping. Our detailed studies reveal that polyzwitterion-based transistors exhibit optoelectronic synaptic behavior with ultralow-power consumption (~250 aJ per spike) and enable high-performance in-sensor reservoir computing, achieving 95.56% accuracy in perceiving the trajectory of moving basketballs.


Replacing electrolyte dielectric with polyzwitterions enables ultralow-power optoelectronic synapse for in-sensor computing.

INTRODUCTION

Driven by Moore’s law, digital artificial intelligence (AI) hardware has undergone rapid development, featuring nanometer-sized transistors and ultrahigh integration density (16). However, digital AI hardware is still far from parallel the efficiency and intelligence of the brain, mainly because of two reasons. First, the huge amount of data shuttling between sensing, processing, and memory units leads to large energy and time overheads. Second, transistor size is close to its physical limit, and technology node scaling is getting increasingly cost ineffective. This is further intensified by the growing complexity of AI applications such as autonomous driving and smart chatbots (111). On the contrary, the human brain features extremely low power consumption (around 20 W), with the energy consumed by a single excitatory spike measuring only 1 fJ (10−15 J) (5, 717), while being able to handle complex problems such as real-time visual recognition, making it an attractive model for developing energy-efficient neuromorphic AI hardware.

To emulate the operation of the human brain, bio-inspired ionic transistor-based artificial synapses have been developed (79, 1221). To date, solid electrolyte dielectrics with mobile free ions, such as LiClO4-doped polyethylene glycol (9, 12, 14, 16), lithium phosphorous oxynitride electrolyte (17), chitosan (15, 16), and others, have been used in transistors to achieve high dielectric capacitances and replicate different synaptic behaviors (8, 1617, 19). Regulating presynaptic input signals, such as magnitude, pulse width, and pulse number, generates diverse synaptic behaviors, including short-term plasticity (STP), long-term plasticity (LTP), spike time-dependent plasticity, and others (2224). In addition, such ionic transistor-based artificial synapses feature colocation of neural signal processing and synaptic weight storage, obviating the von Neumann bottleneck. Despite their promise, these solid electrolyte transistors still face several challenges: (i) The mobile free ions would cause a large leakage current between the gate and source/drain electrodes due to long-range ion migrations, which notably increases the static power consumption (2530); (ii) the high electric fields pose a potential risk of electrolysis (28); (iii) the irreversible synaptic potentiation may result from permanent ion trapping or semiconductor doping (9, 12, 17, 31); (iv) transistors based on these electrolyte dielectrics generally poorly respond to light irradiation due to “exciton-polaron quenching”, disqualifying them as in-sensor neuromorphic vision devices (Fig. 1) (32).

Fig. 1. The advantages of polyzwitterion dielectric in transistor-based artificial synaptic devices.

Fig. 1.

The ions in conventional electrolyte dielectric can move freely and contribute to high leakage. The ions in polyzwitterion dielectric are linked by alkyl chain and can well suppress the leakage current.

To address the challenges outlined above, we propose a previously unreported electrolyte design strategy that covalently connects the cation and anion via a flexible alkyl chain, specifically poly (sulfobetaine methacrylate) (PSBMA). This design eliminates the long-range migration of free ions during polarization while maintaining well-defined polarization-relaxation behaviors under different applied presynaptic inputs (Fig. 1). In addition, polyzwitterions exhibit high capacitance (up to 2000 nF cm−2 @20 Hz) and permittivity (k ~ 165), enabling low operation voltage and thus low power consumption (~250 aJ per spike) in synaptic transistors. Furthermore, PSBMA induces pronounced photoresponse in the transistor via an “interfacial trapping” strategy. The well-defined polarization-relaxation behaviors of polyzwitterions render the resulting transistors unprecedently rich optoelectrical synaptic behaviors, including excitatory postsynaptic current (EPSC), paired-pulse facilitation (PPF), STP, LTP, short-term memory (STM), and long-term memory (LTM), making it suitable for image sensing, storage, and real-time preprocessing (3340). Leveraging these advantages, this artificial synapse enables high-performance in-sensor reservoir computing (RC), achieving 95.56% accuracy in perceiving the trajectory of a moving basketball. Furthermore, the excellent water solubility of polyzwitterion-based flexible devices ensures their degradation upon demand (41), reducing the possibility of e-waste. This work represents an example of opto-neuromorphic computing based on electrolyte dielectrics–based transistors and provides a design for flexible, eco-friendly, and ultralow-power artificial synapses, paving the way for highly efficient edge neuromorphic computing.

RESULTS

Characterization of PSBMA dielectrics

The chemical structure of PSBMA and its capacitor architecture are shown in Fig. 2A. PSBMA has a large dipole moment (~16 D) (41), resulting in a large capacitance of up to 2000 nF cm−2 at 20 Hz and a dielectric permittivity of 165. Its capacitance remains high even at a high frequency of 10,000 Hz (Fig. 2B), outperforming conventional solid electrolyte dielectrics that drastically decrease their capacitances over frequency and lose over 95% capacitance under identical conditions. Moreover, the lack of mobile free ions in PSBMA chains brings down the conductivity and leakage current to a much lower value than that of solid electrolytes (Fig. 2, C and E), which is critical to reducing static power consumption in synaptic devices. The low leakage current and higher capacitance make PSBMA dielectrics highly suitable for constructing low-power devices. Thermogravimetric analysis demonstrates that PSBMA film has good thermal stability, with only a 5% weight loss at 278°C (fig. S2A). Differential scanning calorimetry confirms the noncrystalline nature of the film (fig. S2B). These features make PSBMA an attractive candidate as a dielectric material in synaptic devices. In addition, the excellent water solubility and flexibility of the PSBMA capacitor enable it to adhere to curved surfaces, such as green leaves, and degrade on demand (Fig. 2D), underscoring its eco-friendly nature. The PSBMA film remains intact in common solvents for device fabrication (fig. S2C), rendering excellent compatibility with the patterning of subsequent semiconducting layers.

Fig. 2. Dielectric properties of PSBMA.

Fig. 2.

(A) Schematic illustration of the chemical structure of PBSMA and the architecture of the capacitor. (B) Capacitance and the dielectric constant of PSBMA films (thickness, 280 nm) at different frequencies. (C) Leakage current density of PSBMA films at different voltages. (D) The demonstration of degradation of the PSBMA capacitor array. (E) Conductivity comparison of solid electrolyte-based dielectric layers and the polyzwitterion dielectric layer (47, 48). All statistical data are presented as a mean ± SD (n = 10).

Characterization of organic field-effect transistors with PSBMA dielectric layer

The three-terminal organic field-effect transistor (OFET) containing a 2-decyl[1]benzothieno[3,2-b][1]benzothiophene (BTBT-C10) semiconducting layer and a PSBMA dielectric layer is shown in Fig. 3A. The source-drain current (Id) reaches 10−4 A at a low operation voltage of −4 V due to the very high capacitance of PSBMA (Fig. 3C and fig. S3). Figure 3B shows a typical output curve of the OFET. The subthreshold swing is only 95 mV/Dec, much lower than the previous reports and very close to the theoretical value of 60 mV/Dec (42), implying that the device could easily turn on. A dual sweep of the transfer curve (Vg sweeps from 0 to −4 V and then back to 0 V) shows an obvious hysteresis loop (fig. S5), manifesting the potential of the OFET as an artificial synapse (4345). The devices show typical hole mobility (μ), threshold voltage (Vth), and on/off ratio of 1.2 cm2 V−1 s−1, −2.1 V, and 106 at −4 V, respectively (Fig. 3C and fig. S4). OFETs bearing other semiconductors [such as Pentacene and N,N′-dioctyl-naphthalene tetracarboxylic diimide (C8-NDI)] also exhibit good electrical performance (fig. S8), indicating the excellent generality of the PSBMA dielectric layer. The above results demonstrate the capability of PSBMA as the dielectric layer for high-performance OFETs. In addition, PSBMA renders the OFET remarkable flexibility. The Id of the flexible OFETs shows negligible decay even after 400 bending cycles with a bending radius of 0.62 cm (Fig. 3D).

Fig. 3. Characterization of PSBMA-based transistors.

Fig. 3.

(A) Schematic illustration of the flexible OFETs with PSBMA dielectrics. (B) The output curve and (C) typical p-type transfer curve of the OFETs with BTBT-C10 as the semiconductor and PSBMA as the dielectric layer (Vd = −2 V). (D) The Id change over bending cycles with a bending radius of 0.62 cm. The statistical data are presented as a mean ± SD (n = 10). (E) The low-power ESPC behavior of the OFETs triggered by a presynaptic spike (Vg = −0.3 V, 28 ms). (F) Comparison of energy consumption of transistors fabricated based on various ionic dielectric layers (4961).

Next, we evaluate the capability of PSBMA-based OFETs as artificial synapses. As shown in Fig. 4, the OFET exhibits a typical EPSC. Upon being triggered by a presynaptic spike (Vg = −2 V, pulse width = 0.2 s), the EPSC showed a peak current value of 13.5 nA and then gradually returned to the baseline (the EPSC was recorded at a constant Vd of −0.05 V; fig. S9). When a pair of identical presynaptic spikes with an interval (Δt) of 0.2 s was applied to the gate electrode, the EPSC triggered by the second presynaptic spike is twice as large as the EPSC triggered by the first spike, which is similar to the phenomenon of PPF observed in biological synaptic systems. According to the equation of energy consumption (Ec)

Ec=Vread×Ipeak×t

where Vread represents the drain voltage, Ipeak represents the spike peak current, and t is the spike duration time. The Ec could be effectively reduced by using a small Vread and short presynaptic spike. In Fig. 3E, the Vread is set to −5 μV with a spike duration time of 28 ms, and the EPSC peak current value is −1.7 nA. On the basis of the equation described above, the Ec per spike is approximately 250 aJ, much lower than that of most reported artificial synapses based on electrolyte-gated OFET (EGOFET) (Fig. 3F). This result indicates the potential for low-energy optoelectronic neuromorphic computing devices.

Fig. 4. Photoresponsive of the flexible OFETs.

Fig. 4.

(A) The net photocurrent of OFETs over Vg after 5- and 10-s light irradiation with an intensity of 4.2 mW cm−2, respectively (n = 10). (B) The transfer curves of transistor under dark conditions, after 5-s light exposure, and after 10-s light exposure, respectively (light intensity of 4.2 mW cm−2, Vd = −2 V). The photocurrent response of the transistor (C) under different pulse widths (light intensity of 0.7 mW cm−2, Vg = Vd = −2 V) and (D) under different light intensities (pulse widths of 4 s, Vg = Vd = −2 V). (E) Id as a function of the light pulse number. The phototransistors are working in a real-time “sampling” mode with a constant Vg and Vd of −2 V. (F) Illustrations of dynamic learning and forgetting of the letter “F” (light intensity of 0.7 mW cm−2). (G) The ESPC behavior of the transistors triggered by a light pulse (intensity: 4.2 mW cm−2, pulse width: 0.3 s, Vd = −1 μV, Vg = −2 V).

Photoresponsive behaviors of the flexible OFETs

Conventional EGOFETs barely respond to light irradiation due to the “exciton-polaron quenching” effect and are therefore unable to serve as neuromorphic retinas, as reported previously (32). However, PSBMA-based OFETs exhibit a notable increase in Id when exposed to light irradiation (more than 50 μA at Vg of −4 V), as illustrated in Fig. 4A (fig. S10). The transfer characteristics of the OFETs after exposure to a light intensity of 4.2 mW cm−2 for 0, 5, and 10 s, respectively, are depicted in Fig. 4B. The Id increases continuously without rapid saturation over the light intensities or pulse widths (Fig. 4, C and D), which is akin to the STP and LTP of the human brain. Furthermore, the detectivity (D*), photo/dark current ratio (P), and photoresponsivity (R) of the OFET are elaborated in fig. S11. The larger the pulse width, the higher the Id of the OFETs, demonstrating the potential for use in neuromorphic retinas. Figure 4E demonstrates that as the presynaptic spike numbers increase, the Id also increases and takes longer to decay, which is a typical process of learning and memory in the human brain where STM is transformed into LTM (fig. S15). These devices could also be reset by clearing the residual photocurrent. As shown in fig. S14, after the light is removed, the photocurrent undergoes a slow decay, but it rapidly recovers upon receiving an electrical pulse (Vg = −2 V, 0.5 s). The device, after reset, is prepared to receive the next sequence of optical pulses and can repeatedly respond to new optical pulses with similar initial photocurrents. These results highlight the robust learning capability of PSBMA-based OFETs. To further demonstrate this capability, we applied a light pulse with an intensity of 4.2 mW cm−2 to a transistor array through a photomask with an “F” pattern. Each transistor corresponds to one image pixel. As shown in Fig. 4F, the irradiated pixels gain a higher Id than the masked pixels, and the longer the irradiation time, the higher the Id of the irradiated pixels. As a result, the letter F is sensed and memorized in the array after removing the light pulse, demonstrating the retina-like signal preprocessing capability of the transistor array. These properties enable the transistor to behave as a photosynapse with a fading memory. In addition, thanks to the high capacitance of the PSBMA layer, the transistor-based photosynapse can also work in a low-power mode. When the transistor is working in a “sampling” mode with a constant Vd of −1 μV under a light irradiation of 0.3 s (4.2 mW cm−2), the Ec is approximately 330 aJ per spike (Fig. 4G). It is important to note that in the calculation of power consumption, we have not accounted for the energy consumption attributed to light irradiation. This approach is consistent with the methodology reported in the literature, ensuring good comparability with previous studies (18, 22, 36).

Mechanism study for the photoresponses and fading memory of OFETs

To gain a deeper understanding of the unique photoresponses and fading memory of the PSBMA-based OFETs, we conducted a morphological study of the dielectric layer and semiconductor film using atomic force microscopy (AFM) and grazing-incidence x-ray diffraction (GIXD). Figure 5 (A and B) displays the respective surface morphology of PSBMA and BTBT-C10 films. The PSBMA film is amorphous and featureless, with a root-mean-square (RMS) value of 0.299 nm. In contrast, the BTBT-C10 film shows a high crystalline feature, along with a higher RMS of 1.39 nm. GIXD characterizations provide additional evidence for the high crystallinity of BTBT-C10. The sharp diffraction spots assigned to the {0 0 l} planes in the out-of-plane direction and the {1 k l} planes along the in-plane direction imply that the BTBT-C10 film has a good long-range order in three-dimensional space. The BTBT-C10 molecules adopt a head-to-head and tail-to-tail packing mode, with a periodic spacing of 43.4 and 3.97 Å along the “Z” and “Y” axis, respectively (Fig. 5F; the Cambridge Crystallographic Data Centre deposition number of BTBT-C10 is 1857063). The excellent molecular ordering in the semiconducting layer indicates that the PSBMA layer does not impede the growth of the BTBT-C10 film, which is crucial for achieving high charge carrier mobilities and on/off ratios, as well as low operation voltages. However, highly ordered semiconductors typically result in poor photoresponses of the transistor, as the photogenerated holes and electrons recombine rapidly in the crystal and thereby quench the photocurrent (46). We observed pronounced photoresponses and fading memory of the transistor in this study (Fig. 4). This could be attributed to the interfacial trapping of the charge carrier between the semiconductor and PSBMA dielectrics. The surface charge trap density of PSBMA is around 10 times higher than that of poly(methyl methacrylate) (PMMA) (see supporting information for details). As shown in Fig. 5 (G and H), upon applying a negative Vg, band bending occurs and the holes are injected into the interface between BTBT-C10 and the PSBMA layer from the source electrode. Concurrently, the polyzwitterions align themselves with anions pointing toward the BTBT-C10 layer and cations away from it. Driven by the Vd, these holes become mobile and form Id. Light irradiation generates more holes at the highest occupied molecular orbital and electrons at the lowest unoccupied molecular orbital of the BTBT-C10, respectively. Part of the holes are trapped by the anions of the polyzwitterions, which slows down the recombination of the electrons and holes, giving rise to a pronounced photocurrent and a fading memory. As a control, OFETs with PMMA dielectrics without ionic traps do not exhibit any fading memory (fig. S13), because the electrons and holes can undergo rapid recombination.

Fig. 5. Characterization of films and mechanism study.

Fig. 5.

AFM characterizations of (A) PSBMA and (B) BTBT-C10 films, respectively. (C) 2D GIXD of BTBT-C10 films, with the out-of-plane diffraction peaks shown in (D), and in-plane diffraction peaks shown in (E). (F) The schematical illustration of molecular packing, ordering, and orientation of BTBT-C10. (G and H) Schematic illustration of the mechanism of photoresponses and fading memory.

Nonlinear mapping of 5-bit input of the OFETs

The above fading memory, or the nonlinear dynamic evolution of channel current upon the light stimulus of PSBMA-based OFETs, is key to in-sensor RC. This approach leverages the inherent photoresponses dynamics of OFETs for feature extraction, followed by a trainable lightweight readout map, suitable for sequence data analysis at a low training cost. To characterize their capability for sequential input embedding, we applied optical pulse trains to the transistor (Fig. 6B and fig. S16). Each optical pulse train contains five pulses, with “1” and “0” representing an optical pulse with light intensity of 70 and 0 μW cm−2, respectively, and a pulse width of 2.0 s. Thanks to the efficient exciton dissociation and hole trapping at the BTBT-C10/PSBMA interface, the Ids increases continuously over consecutive light pulses, rather than rapidly saturating. After the light is removed, the trapped holes at the BTBT-C10/PSBMA interface slowly recombine with the free electrons, resulting in a nonlinear decay of the output Id and thus a STM. Therefore, the combined effect of photogating and fading memory enables synaptic facilitation/depression and dynamic transistor states with well-separated outputs, mimicking the synapses of visual signal pathway. As shown in Fig. 6C, 32 optical pulse trains ranging from (00000) to (11111) generate 32 clearly distinguishable states, highlighting the robust ability to map complicated spatiotemporal signals into reservoir states.

Fig. 6. Nonlinear mapping of 5-bit input of the OFETs.

Fig. 6.

(A) Schematical illustration of biological synapse and neural network. (B) Illustration of optical pulse trains applied to the OFETs and the process of RC. (C) Experimental outputs of 32 different 5-bit optical pulse trains, ranging from (00000) to (11111). Each data point represents the average of 10 repeated tests (n = 10).

In-sensor RC for motion recognition

The experimental results about photoresponses to 5-bit sequential optical spikes, presented in Fig. 6C, demonstrate the potential of OFETs photosynapses for in-sensor RC. Grouping OFETs into a pixel array, we propose using the in-sensor reservoir for motion recognition, as illustrated in Fig. 7A. The reservoir maps complex inputs to reservoir states for feature extraction and the linear output layer uses these features for classification. RC has the advantage of minimal training; specifically, the input and reservoir layers remain static, while only the weight of the linear output layer needs to be trained. This renders it well suited for edge learning applications.

Fig. 7. In-sensor RC system for basketball motion recognition.

Fig. 7.

(A) Schematic illustration of the RC system for classifying the basketball motion. (B) The photonic synapse array for mapping spatiotemporal vision information. Each shooting event is divided into five sequential frames (Ft4, Ft3, Ft2, Ft1, and Ft0), representing five distinct moments during ball movement. (C) Schematic illustration of the trajectory of basketball in five different states. (D) Confusion matrix for categorizing various basketball shooting actions. (E) Performance of the RC network over epochs. The blue and pink dots correspond to the classification accuracy of the software and our device-based RC system, respectively. (F) Dimensionality reduction of the reservoir outputs using linear discriminant analysis (LDA). (G) The number of training operations for RC, artificial neural network (ANN) without hidden layers and with one hidden layer, respectively, showing RC notably reduces the training complexity. (H) Initial/final conductance distributions before/after training.

The in-sensor reservoir captured basketball shooting trajectories using a customized dataset comprising five representative classes: up, down, left, right, and middle, shown in Fig. 7C. To integrate spatial and temporal information from successive frames into compact representations, we divided each shooting into five sequential frames (Ft4, Ft3, Ft2, Ft1, and Ft0), representing five distinct moments during ball movement, as shown in Fig. 7B. For each pixel, its temporal evolution is reduced to a 5-bit sequence, s(t), consisting of 32 possible binary vectors encoded as light intensities. The photosynapses of the pixel array, where individual transistors produce features (conductance) corresponding to one of the 32 unique illumination patterns (shown in Fig. 6C). By doing so, temporal pixel evolutions are embedded into the conductance of individual phototransistors, which are concatenated to represent the temporal feature of the video.

The readout map is a trainable classification head for the extracted features by the photosynapse, which is a fully connected layer here. As shown in Fig. 7D, the confusion matrix for categorizing various basketball shootings exhibited dominant diagonal elements, indicating high accuracy within each category. Our training outcomes are detailed in Fig. 7E, with an overall simulated accuracy of 95.56% based on electrically characterized device behaviors as depicted by red dots, matching the performance of the software baseline using the one-layer fully connected neural network (blue dots). Noise experiments further confirm that the 32 states are clearly distinguishable (fig. S17). Figure 7H displays the evolution of both initial and final weight distributions throughout the readout layer. In Fig. 7F, we present the two-dimensional clustering of OFET photosynapse extracted feature vectors using linear discriminant analysis (LDA) for dimensionality reduction. In this representation, distinct shooting states are denoted by spheres of varying colors, while the “x” and “y” axes correspond to the new two-dimensional feature vector after dimensionality reduction. The figure demonstrates clear differentiation among the five shooting states. These features undergo effective nonlinear transformations owing to the STMs of the PSBMA-based OFETs. Last, Fig. 7G compares the number of training parameters required for a RC system, a single-layer fully connected neural network, and a two-layer fully connected neural network. We observe that the number of parameters demanded for a deep fully connected network grows rapidly, while this quantity remains fixed for the RC system. This highlights the advantages of RC for cost-effective real-time edge learning, given its capacity for maintaining manageable complexity even when depth increases.

DISCUSSION

To address the challenges associated with conventional solid electrolyte dielectrics–based artificial synapses, such as high-power consumption and poor responses to light, we proposed a previously unreported electrolyte design strategy. This strategy involves covalently connecting the cation and anion with a flexible alkyl chain (i.e., PSBMA) to eliminate the long-range migration of free ions during polarization while maintaining well-defined polarization-relaxation behaviors under different applied presynaptic inputs. The resulting polyzwitterions exhibit a high capacitance (up to 2000 nF cm−2 @20 Hz) and permittivity (k ~ 165), enabling low operation voltage and low power consumption (~250 aJ per spike) for the synaptic transistors. In addition, PSBMA induces a pronounced photoresponse of the transistor via an interfacial trapping strategy. Furthermore, the transistor exhibits unprecedently rich optoelectrical synaptic behaviors, including EPSC, PPF, STP, LTP, STM, and LTM, making it capable for image sensing, memorization, and real-time preprocessing. Leveraging these behaviors, this artificial synapse serves as an in-sensor reservoir, which is capable of perceiving the trajectory of a moving basketball with an accuracy of 95.56%. Furthermore, because of its excellent water solubility, the polyzwitterion-based flexible devices can degrade upon demand, eliminating the possibility of e-waste. This work represents an example of opto-neuromorphic computing based on electrolyte dielectrics–based transistor and provides a design for flexible, eco-friendly, and ultralow-power artificial synapses, paving the way for highly efficient neuromorphic computing.

MATERIALS AND METHODS

Simulation of the in-sensor RC system for basketball motion recognition

Initially, 25 shots were taken for each class, resulting in a total of 125 records captured via video footage. We selected five consecutive frames from each recording to create a dataset, and each frame was resized to 150 × 150 pixels before being binarized. To form the dataset for the simulated in-sensor RC system, we merged the five frames of each shot in chronological order to create a 22,500 × 5 matrix, where the pulse sequence of each row corresponds to one of the 32 illumination patterns (“00000” to “11111”). The in-sensor RC system consists of 22,500 optically operated memory devices serving as the reservoir nodes, with the conductance programming of these memory devices tuned on the basis of experimental measurements obtained from individual devices. We used a fully connected readout layer with 22,500 inputs (corresponding to the reservoir nodes) and five output neurons representing the different basketball classes (“up”, “down”, “left”, “right”, and “middle”). The readout layer was implemented via software, and we trained the model by minimizing categorical cross-entropy loss using gradient descent optimized with the Adam algorithm (with an initial learning rate set at 0.0001). The total number of training epochs was set to 150. Last, we divided the data into training and test sets, with 80 groups reserved for training and 45 for evaluating the model’s performance.

Acknowledgments

Funding: This work was supported by the following: the National Natural Science Foundation of China [22275193 (W.H.)]; the Natural Science Foundation of Fujian Province [2021 J06034 (W.H.)]; Self-deployment Project Research Program of Haixi Institutes, Chinese Academy of Science, CXZX-2022-GH09 [E255KF0101 (W.H.)]; Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences [E055AJ0101 (W.H.)]; HK RGC (grant nos. 27206321, 17205922, and 17212923 (Z.W.)]; NSFC [grant no. 62122004 (Z.W.)]; and the National Key R&D Program of China [grant no. SQ2022YFB3600159 (Z.W.)]. This research is also partially supported by ACCESS–AI Chip Center for Emerging Smart Systems, sponsored by Innovation and Technology Fund (ITF), Hong Kong SAR.

Author contributions: X.W. conducted the experiments and data visualization. S.S. performed the in-sensor RC. W.H. and Z.W. initiated the idea and wrote the manuscript. All authors contributed to the data analyses.

Competing interests: The authors declare that they have no competing interests.

Data and materials availability: All data needed to evaluate the conclusions in the paper are present in the paper and/or the Supplementary Materials.

Supplementary Materials

This PDF file includes:

Supplementary Text

Figs. S1 to S21

References

sciadv.adn4524_sm.pdf (5.1MB, pdf)

REFERENCES AND NOTES

  • 1.Qiu C., Xiao Z., Yang Y., Zhong D., Peng L., Scaling carbon nanotube complementary transistors to 5-nm gate lengths. Science 355, 271–276 (2017). [DOI] [PubMed] [Google Scholar]
  • 2.Yao P., Wu H., Gao B., Tang J., Zhang Q., Zhang W., Yang J., Qian H., Fully hardware-implemented memristor convolutional neural network. Nature 577, 641–646 (2020). [DOI] [PubMed] [Google Scholar]
  • 3.Ma C., Luo Z., Huang W., Zhao L., Chen Q., Lin Y., Liu X., Chen Z., Liu C., Sun H., Jin X., Yin Y., Li X., Sub-nanosecond memristor based on ferroelectric tunnel junction. Nat. Commun. 11, 1439 (2020). [DOI] [PMC free article] [PubMed] [Google Scholar]
  • 4.Xia Q., Yang J., Memristive crossbar arrays for brain-inspired computing. Nat. Mater. 18, 309–323 (2019). [DOI] [PubMed] [Google Scholar]
  • 5.Lu Y., Liu K., Yang J., Zhang T., Cheng C., Dang B., Xu L., Zhu J., Huang Q., Huang R., Yang Y., Highly uniform two-terminal artificial synapses based on polycrystalline Hf0.5Zr0.5O2 for sparsified back propagation networks. Adv. Electron. Mater. 6, 2000204 (2020). [Google Scholar]
  • 6.Luo J., Liu T., Fu Z., Wei X., Yang M., Chen L., Huang Q., Huang R., A novel ferroelectric FET-based adaptively-stochastic neuron for stimulated-annealing based optimizer with ultra-low hardware cost. IEEE. Electron. Device. Lett. 43, 308–311 (2022). [Google Scholar]
  • 7.Wang T., Meng J., He Z., Chen L., Zhu H., Sun Q., Ding S., Zhou P., Zhang D., Ultralow power wearable heterosynapse with photoelectric synergistic modulation. Adv. Sci. 7, 1903480 (2020). [DOI] [PMC free article] [PubMed] [Google Scholar]
  • 8.Fuller E. J., Keene S. T., Melianas A., Wang Z., Agarwal S., Li Y., Tuchman Y., James C. D., Marinella M. J., Yang J., Salleo A., Talin A. A., Parallel programming of an ionic floating-gate memory array for scalable neuromorphic computing. Science 364, 570–574 (2019). [DOI] [PubMed] [Google Scholar]
  • 9.Xu W., Min S., Hwang H., Lee T. W., Organic core-sheath nanowire artificial synapses with femtojoule energy consumption. Sci. Adv. 2, 1501326 (2016). [DOI] [PMC free article] [PubMed] [Google Scholar]
  • 10.Wu C., Huang Q., Zhao Y., Wang J., Wang Y., Huang R., Design guideline for complementary heterostructure tunnel FETs with steep slope and improved output behavior. IEEE. Electron. Device. Lett. 37, 20–23 (2016). [Google Scholar]
  • 11.Wu C., Huang Q., Zhao Y., Wang J., Wang Y., Huang R., A novel tunnel FET design with stacked source configuration for average subthreshold swing reduction. IEEE Trans. Electron Devices 63, 5072–5076 (2016). [Google Scholar]
  • 12.Sharbati M. T., Du Y., Torres J., Ardolino N. D., Yun M., Xiong F., Low-power, electrochemically tunable graphene synapses for neuromorphic computing. Adv. Mater. 30, e1802353 (2018). [DOI] [PubMed] [Google Scholar]
  • 13.Tian H., Cao X., Xie Y., Yan X., Kostelec A., DiMarzio D., Chang C., Zhao L., Wu W., Tice J., Cha J., Guo J., Wang H., Emulating bilingual synaptic response using a junction-based artificial synaptic device. ACS Nano 11, 7156–7163 (2017). [DOI] [PubMed] [Google Scholar]
  • 14.Zhu J., Yang Y., Jia R., Liang Z., Zhu W., Rehman Z. U., Bao L., Zhang X., Cai Y., Song L., Huang R., Ion gated synaptic transistors based on 2D van der waals crystals with tunable diffusive dynamics. Adv. Mater. 30, e1800195 (2018). [DOI] [PubMed] [Google Scholar]
  • 15.Liu Y., Zhu L., Feng P., Shi Y., Wan Q., Freestanding artificial synapses based on laterally proton-coupled transistors on chitosan membranes. Adv. Mater. 27, 5599–5604 (2015). [DOI] [PubMed] [Google Scholar]
  • 16.He Y., Nie S., Liu R., Jiang S., Shi Y., Wan Q., Spatiotemporal information processing emulated by multiterminal neuro-transistor networks. Adv. Mater. 31, e1900903 (2019). [DOI] [PubMed] [Google Scholar]
  • 17.Fuller E. J., Gabaly F. E., Leonard F., Agarwal S., Plimpton S. J., Jacobs-Gedrim R. B., James C. D., Marinella M. J., Talin A. A., Li-ion synaptic transistor for low power analog computing. Adv. Mater. 29, 1604310 (2017). [DOI] [PubMed] [Google Scholar]
  • 18.Yang B., Lu Y., Jiang D., Li Z., Zeng Y., Zhang S., Ye Y., Liu Z., Ou Q., Wang Y., Dai S., Yi Y., Huang J., Bioinspired multifunctional organic transistors based on natural chlorophyll/organic semiconductors. Adv. Mater. 32, e2001227 (2020). [DOI] [PubMed] [Google Scholar]
  • 19.Zhou J., Liu N., Zhu L., Shi Y., Wan Q., Energy-efficient artificial synapses based on flexible IGZO electric-double-layer transistors. IEEE. Electron. Device. Lett. 36, 198–200 (2015). [Google Scholar]
  • 20.Zhu Y., Shin B., Liu G., Shan F., Electrospun ZnSnO nanofibers for neuromorphic transistors with ultralow energy consumption. IEEE. Electron. Device. Lett. 40, 1776–1779 (2019). [Google Scholar]
  • 21.Zhu L., Wan C., Guo L., Shi Y., Wan Q., Artificial synapse network on inorganic proton conductor for neuromorphic systems. Nat. Commun. 5, 3158 (2014). [DOI] [PubMed] [Google Scholar]
  • 22.Liang K., Wang R., Huo B., Ren H., Li D., Wang Y., Tang Y., Chen Y., Song C., Li F., Ji B., Wang H., Zhu B., Fully printed optoelectronic synaptic transistors based on quantum dot-metal oxide semiconductor heterojunctions. ACS Nano 16, 8651–8661 (2022). [DOI] [PubMed] [Google Scholar]
  • 23.Islam M. M., Krishnaprasad A., Dev D., Martinez-Martinez R., Okonkwo V., Wu B., Han S. S., Bae T. S., Chung H. S., Touma J., Jung Y., Roy T., Multiwavelength optoelectronic synapse with 2D materials for mixed-color pattern recognition. ACS Nano 16, 10188–10198 (2022). [DOI] [PubMed] [Google Scholar]
  • 24.Wu X., Dai D., Ling Y., Chen S., Huang C., Feng S., Huang W., Organic single-crystal transistor with unique photo responses and its application as light-stimulated synaptic devices. ACS Appl. Mater. Interfaces 12, 30627–30634 (2020). [DOI] [PubMed] [Google Scholar]
  • 25.Claro P. I. C., Cunha I., Paschoalin R. T., Gaspar D., Miranda K., Oliveira O. N. Jr., Martins R., Pereira L., Marconcini J. M., Fortunato E., Mattoso L. H. C., Ionic conductive cellulose mats by solution blow spinning as substrate and a dielectric interstrate layer for flexible electronics. ACS Appl. Mater. Interfaces 13, 26237–26246 (2021). [DOI] [PubMed] [Google Scholar]
  • 26.Yin Z., Yin M., Liu Z., Zhang Y., Zhang A., Zheng Q., Solution-processed bilayer dielectrics for flexible low-voltage organic field-effect transistors in pressure-sensing applications. Adv. Sci. 5, 1701041 (2018). [DOI] [PMC free article] [PubMed] [Google Scholar]
  • 27.Dai S., Chu Y., Liu D., Cao F., Wu X., Zhou J., Zhou B., Chen Y., Huang J., Intrinsically ionic conductive cellulose nanopapers applied as all solid dielectrics for low voltage organic transistors. Nat. Commun. 9, 2737 (2018). [DOI] [PMC free article] [PubMed] [Google Scholar]
  • 28.Choi J. H., Xie W., Gu Y., Frisbie C. D., Lodge T. P., Single ion conducting, polymerized ionic liquid triblock copolymer films: High capacitance electrolyte gates for n-type transistors. ACS Appl. Mater. Interfaces 7, 7294–7302 (2015). [DOI] [PubMed] [Google Scholar]
  • 29.Petritz A., Wolfberger A., Fian A., Irimia-Vladu M., Haase A., Gold H., Rothländer T., Griesser T., Stadlober B., Cellulose as biodegradable high-kdielectric layer in organic complementary inverters. Appl. Phys. Lett. 103, 153303 (2013). [Google Scholar]
  • 30.Yang Y., Wen J., Guo L., Wan X., Du P., Feng P., Shi Y., Wan Q., Long-term synaptic plasticity emulated in modified graphene oxide electrolyte gated IZO-based thin-film transistors. ACS Appl. Mater. Interfaces 8, 30281–30286 (2016). [DOI] [PubMed] [Google Scholar]
  • 31.Wang Z., Chen X., Yu L., Guo S., Hu Y., Huang Y., Wang S., Qi J., Han C., Ma X., Zhang X., Dong H., Chen W., Li L., Hu W., Polymer electrolyte dielectrics enable efficient exciton-polaron quenching in organic semiconductors for photostable organic transistors. ACS Appl. Mater. Interfaces 14, 13584–13592 (2022). [DOI] [PubMed] [Google Scholar]
  • 32.Wu X., Wang S., Huang W., Dong Y., Wang Z., Huang W., Wearable in-sensor reservoir computing using optoelectronic polymers with through-space charge-transport characteristics for multi-task learning. Nat. Commun. 14, 468 (2023). [DOI] [PMC free article] [PubMed] [Google Scholar]
  • 33.Tan H., van Dijken S., Dynamic machine vision with retinomorphic photomemristor-reservoir computing. Nat. Commun. 14, 2169 (2023). [DOI] [PMC free article] [PubMed] [Google Scholar]
  • 34.Liu X., Sun C., Guo Z., Xia X., Jiang Q., Ye X., Shang J., Zhang Y., Zhu X., Li R., Near-sensor reservoir computing for gait recognition via a multi-gate electrolyte-gated transistor. Adv. Sci. 10, 2300471 (2023). [DOI] [PMC free article] [PubMed] [Google Scholar]
  • 35.Liu K., Zhang T., Dang B., Bao L., Xu L., Cheng C., Yang Z., Huang R., Yang Y., An optoelectronic synapse based on α-In2Se3 with controllable temporal dynamics for multimode and multiscale reservoir computing. Nat. Electron. 5, 761–773 (2022). [Google Scholar]
  • 36.Lao J., Yan M., Tian B., Jiang C., Luo C., Xie Z., Zhu Q., Bao Z., Zhong N., Tang X., Sun L., Wu G., Wang J., Peng H., Chu J., Duan C., Ultralow-power machine vision with self-powered sensor reservoir. Adv. Sci. 9, 2106092 (2022). [DOI] [PMC free article] [PubMed] [Google Scholar]
  • 37.Zhong Y., Tang J., Li X., Gao B., Qian H., Wu H., Dynamic memristor-based reservoir computing for high-efficiency temporal signal processing. Nat. Commun. 12, 408 (2021). [DOI] [PMC free article] [PubMed] [Google Scholar]
  • 38.Wang S., Chen X., Zhao C., Kong Y., Lin B., Wu Y., Bi Z., Xuan Z., Li T., Li Y., Zhang W., Ma E., Wang Z., Ma W., An organic electrochemical transistor for multi-modal sensing, memory and processing. Nat. Electron. 6, 281–291 (2023). [Google Scholar]
  • 39.Chen J., Zhou Z., Kim B. J., Zhou Y., Wang Z., Wan T., Yan J., Kang J., Ahn J. H., Chai Y., Optoelectronic graded neurons for bioinspired in-sensor motion perception. Nat. Nanotechnol. 18, 882–888 (2023). [DOI] [PubMed] [Google Scholar]
  • 40.Chen S., Huang W., Yang K., Xu Y., Wang D., Huang W., Constructing versatile hydrophilic surfaces via in-situ aminolysis. Chin. J. Struc. Chem. 11, 1525–1534 (2021). [Google Scholar]
  • 41.Lee H., Puodziukynaite E., Zhang Y., Stephenson J. C., Richter L. J., Fischer D. A., DeLongchamp D. M., Emrick T., Briseno A. L., Poly(sulfobetaine methacrylate)s as electrode modifiers for inverted organic electronics. J. Am. Chem. Soc. 137, 540–549 (2015). [DOI] [PubMed] [Google Scholar]
  • 42.Ji D., Li T., Zou Y., Chu M., Zhou K., Liu J., Tian G., Zhang Z., Zhang X., Li L., Wu D., Dong H., Miao Q., Fuchs H., Hu W., Copolymer dielectrics with balanced chain-packing density and surface polarity for high-performance flexible organic electronics. Nat. Commun. 9, 2339 (2018). [DOI] [PMC free article] [PubMed] [Google Scholar]
  • 43.Huang C., Feng S., Huang W., Pendant group effect of polymeric dielectrics on the performance of organic thin film transistors. Chin. J. Struc. Chem. 40, 1541–1549 (2021). [Google Scholar]
  • 44.Wu X., Feng S., Shen J., Huang W., Li C., Li C., Sui Y., Huang W., Nonvolatile transistor memory based on a High-kDielectric polymer blend for multilevel data storage, encryption, and protection. Chem. Mater. 32, 3641–3650 (2020). [Google Scholar]
  • 45.Wu X., Dai D., Huang W., Feng S., Huang W., High-k polymer dielectrics with different cross-linked networks for nonvolatile transistor memory device. Org. Electron. 96, 106222 (2021). [Google Scholar]
  • 46.Liu J., Jiang L., Shi J., Li C., Shi Y., Tan J., Li H., Jiang H., Hu Y., Liu X., Yu J., Wei Z., Jiang L., Hu W., Relieving the photosensitivity of organic field-effect transistors. Adv. Mater. 32, 1906122 (2019). [DOI] [PubMed] [Google Scholar]
  • 47.Amanchukwu C. V., Yu Z., Kong X., Qin J., Cui Y., Bao Z., A new class of ionically conducting fluorinated ether electrolytes with high electrochemical stability. J. Am. Chem. Soc. 142, 7393–7403 (2020). [DOI] [PubMed] [Google Scholar]
  • 48.Tybrandt K., Forchheimer R., Berggren M., Logic gates based on ion transistors. Nat. Commun. 3, 871 (2012). [DOI] [PubMed] [Google Scholar]
  • 49.Liu L., Cui B., Xu W., Ni Y., Zhang S., Xu W., Highly aligned indium zinc oxide nanowire-based artificial synapses with low-energy consumption. J. Ind. Eng. Chem. 88, 111–116 (2020). [Google Scholar]
  • 50.Guo L., Zhang G., Han H., Hu Y., Cheng G., Artificial neuron synaptic realization of one device with transparent and environmentally friendly materials. J. Phys. Chem. C 126, 7791–7798 (2022). [Google Scholar]
  • 51.Liu D., Shi Q., Dai S., Huang J., The design of 3D-interface architecture in an ultralow-power, electrospun single-fiber synaptic transistor for neuromorphic computing. Small 16, e1907472 (2020). [DOI] [PubMed] [Google Scholar]
  • 52.Zhang C., Wang S., Zhao X., Yang Y., Tong Y., Zhang M., Tang Q., Liu Y., Sub-femtojoule-energy-consumption conformable synaptic transistors based on organic single-crystalline nanoribbons. Adv. Funct. Mater. 31, 2007894 (2020). [Google Scholar]
  • 53.Gong J., Yu H., Zhou X., Wei H., Ma M., Han H., Zhang S., Ni Y., Li Y., Xu W., Lateral artificial synapses on hybrid perovskite platelets with modulated neuroplasticity. Adv. Funct. Mater. 30, 2005413 (2020). [Google Scholar]
  • 54.Yao B., Li J., Chen X., Yu M., Zhang Z., Li Y., Lu T., Zhang J., Non-volatile electrolyte-gated transistors based on Graphdiyne/MoS2with robust stability for low-power neuromorphic computing and logic-in-memory. Adv. Funct. Mater. 31, 2100069 (2021). [Google Scholar]
  • 55.Hu W., Jiang J., Xie D., Liu B., Yang J., He J., Proton-electron-coupled MoS2synaptic transistors with a natural renewable biopolymer neurotransmitter for brain-inspired neuromorphic learning. J. Mater. Chem. C. 7, 682–691 (2019). [Google Scholar]
  • 56.Dai S., Wang Y., Zhang J., Zhao Y., Xiao F., Liu D., Wang T., Huang J., Wood-derived nanopaper dielectrics for organic synaptic transistors. ACS Appl. Mater. Interfaces 10, 39983–39991 (2018). [DOI] [PubMed] [Google Scholar]
  • 57.Yang J., Ge C., Du J., Huang H., He M., Wang C., Lu H., Yang G., Jin K., Artificial synapses emulated by an electrolyte-gated tungsten-oxide transistor. Adv. Mater. 30, e1801548 (2018). [DOI] [PubMed] [Google Scholar]
  • 58.He Y., Sun J., Qian C., Kong L., Gou G., Li H., Oxide-based synaptic transistors gated by solution-processed gelatin electrolytes. Appl. Phys. A-Mater. 123, 227 (2017). [Google Scholar]
  • 59.Liu R., Zhu L., Wang W., Hui X., Liu Z., Wan Q., Biodegradable oxide synaptic transistors gated by a biopolymer electrolyte. J. Mater. Chem. C. 4, 7744–7750 (2016). [Google Scholar]
  • 60.Balakrishna P. P., Souza M. M. D., Nanoionics-based three-terminal synaptic device using zinc oxide. ACS Appl. Mater. Interfaces 9, 1609–1618 (2017). [DOI] [PubMed] [Google Scholar]
  • 61.Li X., Yu B., Wang B., Bao L., Zhang B., Li H., Yu Z., Zhang T., Yang Y., Huang R., Wu Y., Li M., Multi-terminal ionic-gated low-power silicon nanowire synaptic transistors with dendritic functions for neuromorphic systems. Nanoscale 12, 16348–16358 (2020). [DOI] [PubMed] [Google Scholar]
  • 62.Chen Q., Li Z., Dong B., Zhou Y., Song B., Zwitter-ionic polymer applied as electron transportation layer for improving the performance of polymer solar cells. Polymers 9, 566 (2017). [DOI] [PMC free article] [PubMed] [Google Scholar]

Associated Data

This section collects any data citations, data availability statements, or supplementary materials included in this article.

Supplementary Materials

Supplementary Text

Figs. S1 to S21

References

sciadv.adn4524_sm.pdf (5.1MB, pdf)

Articles from Science Advances are provided here courtesy of American Association for the Advancement of Science

RESOURCES