Open Access Article
Ryoma
Hayakawa
*a,
Yuho
Yamamoto
ab,
Kosuke
Yoshikawa
ab,
Yoichi
Yamada
b and
Yutaka
Wakayama
*a
aResearch Center for Materials Nanoarchitectonics (MANA), National Institute for Materials Science (NIMS), 1-1 Namiki, Tsukuba 305-0044, Japan. E-mail: WAKAYAMA.Yutaka@nims.go.jp; Tel: +81-29-860-4403
bFaculty of Pure and Applied Sciences, University of Tsukuba 1-1-1 Tennodai, Tsukuba 305-8573, Japan
First published on 12th June 2025
Neuromorphic computing, a nonvon Neumann architecture, holds promise for low-power, high-efficiency data processing. Herein, we demonstrated reconfigurable artificial synapses using a floating-gate-type organic antiambipolar transistor (FG-OAAT) to mimic biological synapses. The FG-OAAT exhibited a Λ-shaped transfer curve with negative differential transconductance. A two-dimensional continuous Au film was used as the floating gate to induce a large peak voltage shift in the Λ-shaped transfer curve by controlling hole- and electron-trapping processes in the floating gate. This feature enabled reconfigurable synaptic operations. Long-term potentiation/depression, excitatory/inhibitory, and paired-pulse facilitation/depression functions were electrically reconfigured by tuning the charge conditions in the floating gate. These versatile synaptic operations were induced by a consistent presynaptic signal, with fixed polarity, applied voltage, and pulse width. These behaviors closely resembled those of biological synapses, highlighting the potential for a brain-like computing architecture that surpasses current von Neumann systems.
Neuromorphic computing systems, a type of non von Neumann architecture, offer a solution for energy-efficient AI.10–12 These systems mimic the brain, which operates with ultralow power consumption (20 W) through parallel data processing.13 Neuromorphic devices integrate logic and memory units, with nonvolatile memories such as magnetic random-access memory and ferroelectric memory widely used.14–17 This device configuration enables extremely low-power consumption and high-speed parallel data processing. In addition, the adoption of pulse-based analog operations, such as spiking neural networks, is expected to drive the evolution of highly energy-efficient AI systems.18–20
Organic transistors with nonvolatile memories are widely employed in neuromorphic applications because of their attractive features, including light weight, flexibility, and biocompatibility.21–24 The recognition of complex images and voice patterns has already been demonstrated.25,26 However, conventional organic transistors usually support only synaptic operations for an input signal because they exhibit unipolar carrier transport.21–24 Meanwhile, biological synapses exhibit diverse responses to identical input signals, with synaptic operations reconfigured by neuromodulatory commands.27–30 Accordingly, the development of reconfigurable artificial synapses is a key challenge in the construction of brain-inspired AI systems. To address this, we demonstrate reconfigurable neuromorphic operations based on a floating-gate-type organic antiambipolar transistor (FG-OAAT).
An OAAT is a heterojunction transistor with at least one p–n junction in the transistor channel, which induces negative differential transconductance and produces a Λ-shaped transfer curve.31–37 The drain current increases and then decreases with increasing gate voltage. This unique carrier transport in OAATs has enabled the creation of logic circuits, including ternary and quaternary inverters, ternary logic-in-memory, and reconfigurable two-input logic circuits.38–43
Herein, we applied OAATs to a reconfigurable artificial synapse, using 2,7-dioctyl[1]benzothieno[3,2-b][1]benzothiophene (C8-BTBT) and PhC2H4-benzo[de]isoquinolino[1,8-gh]quinolone diimide (PhC2-BQQDI) films as the p-type and n-type transistor channels, respectively. Notably, a Au film was introduced as the floating gate (FG) to induce a large peak voltage shift in the Λ-shaped transfer curve by controlling the hole- and electron-trapping processes in the FG. This feature enabled unique synaptic operations, with long-term potentiation (LTP)/depression (LTD), excitatory/inhibitory, and paired-pulse facilitation (PPF)/depression (PPD) electrically reconfigured by adjusting the charge conditions of the Au FG. These findings suggest the potential to realize a new computing architecture beyond the current von Neumann computing.
000) layer was spin-coated on the HfO2 surface. Subsequently, C8-BTBT (13 ± 3 nm) and PhC2-BQQDI (8 ± 2 nm) films were grown as p- and n-type organic channels, respectively, via thermal vacuum deposition at a background pressure of 10−7 Pa. Finally, 30 nm-thick Au films were deposited for the source (S) and drain (D) electrodes via thermal vacuum deposition, with typical width and length dimensions of 400 and 200 μm, respectively.
In our previous study, the Λ-shaped transfer curves in OAATs were interpreted analogously to the shoot-through current in complementary metal-oxide-semiconductor inverters. Namely, ID of FG-OAATs is the overlapped current of the constituent n-type and p-type transistors described using the following equations:44–47
![]() | (1) |
![]() | (2) |
Based on the above argument, the carrier transport process in FG-OAATs can be explained using the illustrations shown in Fig. 1e and f. In VBG < Von region (Fig. 1e), no electron current flows because VBG is below the Vth,n of the PhC2-BQQDI channel. However, holes accumulate in the C8-BTBT channel owing to the applied effective gate voltage (VD–VBG). However, the hole current is suppressed by the potential barrier at the p–n junction, resulting in no ID in the VBG range. In VBG > Von (Fig. 1f), electrons are introduced from the S electrode and flow toward the D electrode. Simultaneously, the accumulated holes in the C8-BTBT channel begin to flow toward the S electrode, generating ID in FG-OAATs. A further increase in VBG (VBG > VoffFig. 1g) hinders ID because the C8-BTBT channel enters the off state.
Next, the Λ-shaped transfer curve in the FG-OAAT can be controlled using the Au FG. Fig. 2a–c illustrate the processes of erasing, electron trapping, and hole trapping. The corresponding ID–VBG curves are depicted in Fig. 2d, where the solid and dotted lines at each state represent the forward and reverse VBG sweeps, respectively. First, the Au FG was grounded to erase the carriers (electrons or holes) in the Au FG, which is defined as the erasing process (Fig. 2a). The resulting ID–VBG curve is exhibited by the black solid and dotted lines in Fig. 2d. Vpeak was estimated at 2.1 V. Then, VBG = 5.0 V was applied for 10 s to trap electrons in the Au FG (Fig. 2b), where the S and D electrodes were grounded. This operation shifted the ID–VBG curve higher VG, as shown by the blue solid and dotted lines in Fig. 2d. Vpeak shifted from 2.1 to 3.1 V. Importantly, no hysteresis was observed in the shifted ID–VBG curve, revealing that the trapped electrons in the Au FG were retained during the VBG sweeps. After the erasing process (Fig. 2a), the opposite BG voltage, VBG = −5.0 V, was applied for 10 s to trap holes in the Au FG (Fig. 2c). As a result, Vpeak shifted to 1.0 V (red solid and dotted line in Fig. 2d). No hysteresis appeared in the ID–VBG curve, similar to the electron-trapped sate. Consequently, the total variation in Vpeak reached 2.1 V by controlling the charge conditions (holes or electrons) in the Au FG. This value is much larger than that observed in our previous study with a zinc-phthalocyanine-core star-shaped polymer (ZnPc-PS4) as the FG.43,48 This improvement in Vpeak shift in this study benefits from using the Au FG.
Fig. 2e shows the retention property of electron- and hole-trapped states, where the potential of the Au FG was monitored. The trapped electrons and holes were retained for at least 1800 s. The switching behavior between the erased and electron-trapped states of the FG-OAATs is depicted in Fig. 2f and g. After 10 switching cycles, the Vpeak positions after the electron-trapping and releasing processes were almost identical.
Based on these nonvolatile memory properties, we applied the FG-OAAT to a neuromorphic device. For synaptic operations with the FG-OAAT, the BG and D electrodes function as the presynaptic input and postsynaptic output terminals, respectively. ID was monitored as the postsynaptic current (PSC). Fig. 3a shows ID–VBG for the erased (black solid line), electron-trapped (blue solid line), and hole-trapped (red solid line) states. As shown in Fig. 3b–d, a variety of synaptic operations were reconfigured by adjusting the initial charge condition in the Au FG. First, Fig. 3b illustrates the transition from LTP to LTD with the FG-OAAT. Prior to this measurement, the initial ID–VBG curve was set to the electron-trapped state (blue solid line in Fig. 3a) by applying a VBG of 5.0 V for 10 s. PSC (ID,read) was monitored at a VG (VG,read) of 1.8 V and VD (VD,read) of 3.0 V. When negative VBG pulses (VBG = −5.0 V, pluse width (Pwidth) = 100 ms) were applied, ID,read started increasing and was maintained even after the VBG pulses were turned off, indicating the LTP operation. Thereafter, ID,read decreased with identical positive VBG pulses (VBG = 5.0 V, Pwidth = 100 ms), corresponding to the LTD operation. Next, the opposite transition from LTD to LTP was observed as shown in Fig. 3c even with identical sequence of presynaptic pulses (VBG = −5.0 V, Pwidth = 100 ms and VBG = 5.0 V, Pwidth = 100 ms) applied to the transistor. The difference of Fig. 3b and c is the initial charge conditions in the Au FG.
In Fig. 3c, the initial ID–VBG curve was set to the erased state (black solid line in Fig. 3a). As a result, the transition from LTD to LTP was induced by applying the same sequence of VBG pulses with the negative-to-positive polarity change. Finally, Fig. 3d shows that the transition from LTP to LTD can be induced by applying only negative VBG pulses (VBG = −5.0, Pwidth = 100 ms) continuously. (VBG = −5 V, Pwidth = 100 ms) (Fig. 3d). Here, the initial ID–VBG curve was set to the electron-trapped state (blue solid line in Fig. 3a).
The abovementioned results clearly reveal that reconfigurable synaptic operations, transitioning from LTP to LTD and vice versa, can be achieved by controlling the initial charge conditions of the Au FG. Such synaptic plasticity has typically not been demonstrated in conventional transistors, which exhibit unipolar carrier transport.21–26 By contrast, biological synapses are known to display different responses to synaptic plasticity under neuromodulatory control, even when the same polarity, applied voltage, and pulse width are applied.27–30 This suggests that our proposed transistor has the potential to truly mimic biological synapses. Notably, the continuous VBG pulse applications in Fig. 3d enabled a smooth transition from LTP to LTD, while a sharp drop in ID,read was observed in Fig. 3b when the VBG pulse polarity was reversed. The nonlinearity coefficients and asymmetric factors of LTP/LTD behaviors were also improved by the continuous VBG pulse applications (Fig. S6 in ESI†). This improvement offers an additional advantage of using our proposed transistor.
In a similar manner to the LTP/LTD behaviors, excitatory/inhibitory and PPF/PPD operations were electrically reconfigured, as shown in Fig. 4. Fig. 4a shows the ID–VBG curves before (black dotted line) and after (black solid line) the application of a negative VBG pulse (VBG = −5 V for 100 ms), where no carriers were accumulated in the Au FG in the initial state (black dotted line). The corresponding variation in ID,read is depicted in Fig. 4b, where ID,read was monitored at VG,read = 1.2 V and VD,read = 3.0 V. A sharp increase in ID,read from 25 to 40 nA was observed by the application of a negative VBG pulse (VBG = −5 V for 100 ms). Importantly, ID,read was maintained at 30 nA after the VBG pulse was turned off, due to the threshold voltage shift induced by the hole-trapping process in the Au FG. This variation in ID,read corresponds to the excitatory synaptic operation. The synaptic plasticity was changed by the presynaptic input pulse. Moreover, the PPF behavior distinctly appeared with the application of double-negative VBG pulses (VBG = −5 V for 100 ms) (Fig. 4c). The FFP ratio (ID,read,change) was calculated using the following equation:
![]() | (3) |
Strikingly, the opposite synaptic behaviors, namely inhibitory and PPD operations, are shown in Fig. 4d–f, even though the same VBG pulses as in Fig. 4a–c were applied to the transistor. First, the ID–VBG curve was set to the red dotted line in Fig. 4d, where holes were trapped in the Au FG. Then, the application of a negative VBG pulse (VBG = −5 V for 100 ms) shifted the transfer curve from the red dotted line to the solid line (Fig. 4d), leading to a reduction in ID,read, as shown in Fig. 4e. Similarly, PPD was obtained by applying the same double-negative VBG pulses as in Fig. 4c. The PPD ratio was varied from −2.5% at Pinterval = 3.5 s to −28.0% at Pinterval = 0.5 s with a reduction in pulse intervals.
As shown, we realized reconfigurable synaptic operations. Namely, LTP/LTD, inhibitory/excitatory, and PPF/PPD operations were electrically reconfigured by adjusting the charging conditions of the Au FG. Such reconfigurable synaptic operations have not been attained in other neuromorphic devices. Conversely, our transistor enables versatile operations without changing the presynaptic signals, similar to biological synapses. Thus, our proposed transistors have the potential to enable brain-like computing architectures, surpassing the limitations of the current von Neumann model.
Footnote |
| † Electronic supplementary information (ESI) available. See DOI: https://doi.org/10.1039/d5tc01712b |
| This journal is © The Royal Society of Chemistry 2025 |