Poly(3-hexylthiophene) Based Organic Electrochemical Transistor Optimized with Chloroform and Its Synaptic Function Emulation
-
摘要: 通过旋涂法制备了有机半导体聚（3-己基噻吩）（P3HT）薄膜，在二氯苯溶剂中引入氯仿对P3HT薄膜进行改性，以改性的P3HT薄膜作为沟道层、离子凝胶作为电解质层制备了有机电化学晶体管（OECT）。通过原子力显微镜、紫外-可见光谱和拉曼光谱探究了氯仿改性对P3HT薄膜粗糙度和分子有序度的影响，采用半导体参数仪研究了氯仿改性对材料电学性能的影响。实验结果表明，氯仿改性降低了P3HT薄膜的粗糙度，提高了分子排列的有序度。氯仿改性后的OECT在−0.5 V和−1 V的电脉冲刺激下呈现显著的神经突触兴奋脉冲电流响应特性，相比于未改性的器件，电导调控幅值分别增加了约2倍和16倍，且延长了其保持特性。基于氯仿改性OECT的人工神经突触网络将MNIST手写数字识别准确率从73.6%提高至92.7%，有望在高性能神经形态计算方面发挥重要作用。Abstract: The organic semiconductor poly(3-hexylthiophene) (P3HT) film prepared by the spin-coating method is optimized by dichlorobenzene (o-DCB) solvent added with chloroform (CF). The organic electrochemical transistor (OECT) is obtained using the optimized P3HT film as the channel layer and ion gel as the electrolyte layer. The effect of CF on the roughness and molecular order of P3HT film has been inverstigated by atomic force microscopy, UV-visible spectroscopy and Raman spectroscopy. The effect of CF optimization on the electrical properties of the material is studied with a semiconductor parametic analyzer. Results show that CF introduction reduces the roughness of P3HT film and improves the order degree of P3HT molecular arrangement. The CF-optimized OECT exhibits significant synaptic excitatory pulse current characteristics under the stimulation of −0.5 V and −1 V electric pulses. Compared to the device without CF optimization, the amplitude of conductance regulation is increased by about twice and 16 times, respectively, along with the improved retention performance. The simulation results show that the accuracy of the neural network based on the CF-optimized OECT in recognizing MNIST（Modified National Institute of Standards and Technology） handwritten digits is increased from 73.6% to 92.7%. This device is expected to play an important role in large-scale neuromorphic computing applications.
-
图 1 基于 P3 HT 的 OECT 的制备流程图
Figure 1. Flow chart of P3 HT-based OECT device fabrication
图 2 (a) o-DCB@P3HT 和(b) o-DCB/CF@P3HT 的 AFM 图像；(c) 两种 P3HT 薄膜的光学显微镜照片
Figure 2. AFM images of (a) o-DCB@P3HT and (b) o-DCB/CF@P3HT; (c) Optical microscope images of the two P3HT films
图 3 o-DCB@P3HT 和(b) o-DCB/CF@P3HT 的紫外-可见光谱； (c) o-DCB@P3HT 和(d) o-DCB/CF@P3HT 的拉曼光谱
Figure 3. UV-Vis spectra of (a) o-DCB@P3HT and (b) o-DCB/CF@P3HT; Raman spectra of (c) o-DCB@P3HT and (d) o-DCB/CF@P3HT
图 4 (a) 基于 P3HT 的 OECT 结构示意图；(b) o-DCB@OECT 和(c) o-DCB/CF@OECT 的转移特性曲线；(d) o- DCB@OECT 和(e) o-DCB/CF@OECT 在−0.5 V 和−1.0 V 电脉冲刺激下的 EPSC；(f) 两种 OECT 在−1.0 V 电压脉冲刺激下的弛豫时间常数
Figure 4. (a) Schematic diagram of OECT based on P3HT; Transfer characteristic curve of (b) o-DCB@OECT and (c) o-DCB/CF@OECT; EPSC of (d) o-DCB@OECT and (e) o-DCB/CF@OECT under −0.5 V and −1.0 V electrical pulse stimulation; (f) Relaxation-time constants of the two OECTs under −1.0 V electrical pulse stimulation
图 5 (a) 基于 P3HT 的 OECT 神经网络的 MNIST 图像识别；基于(b) o-DCB@OECT 和(c) o-DCB/CF@OECT 的识别混淆矩阵图；(d) 两种 OECT 网络的识别准确率对比
Figure 5. (a) A neural network based on P3HT@OECT for MNIST image recognition; Identification confusion matrix diagram based on the (b) o-DCB@OECT and (c) o-DCB/CF@OECT; (d) Comparison of the recognition accuracy for the networks based on the two OECTs
-
[1] KIM S J, JEONG J S, JANG H W, YI H, YANG H, JU H, LIM J A. Dendritic network implementable organic neurofiber transistors with enhanced memory cyclic endurance for spatiotemporal iterative learning [J]. Advanced Materials,2021,33(26):2100475. [2] KIM Y, CHORTOS A, XU W, LIU Y, OH J Y, SON D, KANG J, FOUDEH A M, ZHU C, LEE Y, NIU S, LIU J, PFATTNER R, BAO Z, LEE T W. A bioinspired flexible organic artificial afferent nerve [J]. Science,2018,360(6392):998-1003. [3] DAI S, ZHAO Y, WANG Y, ZHANG J, FANG L, JIN S, SHAO Y, HUANG J. Recent advances in transistor-based artificial synapses [J]. Advanced Functional Materials,2019,29(42):1903700. [4] RIVNAY J, INAL S, SALLEO A, OWENS R M, BERGGREN M, MALLIARAS G G. Organic electrochemical transistors [J]. Nature Reviews Materials,2018,3(2):17086. [5] 竺立强. 电解质调控场效应晶体管及其人造突触器件应用 [J]. 中国材料进展,2017,36(10):742-755. doi: 10.7502/j.issn.1674-3962.2017.10.08ZHU L Q. Electrolyte gated field-effect transistors and artificial synaptic device applications [J]. Materials China,2017,36(10):742-755. doi: 10.7502/j.issn.1674-3962.2017.10.08 [6] LENZ J, deL GIUDICE F, GEISENHOF F R, WINTERER F, WEITZ R T. Vertical, electrolyte-gated organic transistors show continuous operation in the MA cm−2 regime and artificial synaptic behaviour [J]. Nature Nanotechnology,2019,14(6):579-585. [7] HUANG J H, YANG C Y, HSU C Y, CHEN C L, LIN L Y, WANG R R, HO K C, CHU C W. Solvent-annealing-induced self-organization of poly(3-hexylthiophene), a high-performance electrochromic material [J]. ACS Applied Materials & Interfaces,2009,1(12):2821-2828. [8] NGUYEN-DANG T, CHAE S, HARRISON K, LLANES L C, YI A, KIM H J, BISWAS S, VISELL Y, BAZAN G C, NGUYEN T Q. Efficient fabrication of organic electrochemical transistors via wet chemical processing [J]. ACS Applied Materials & Interfaces,2022,14(10):12469-12478. [9] SEO D G, LEE Y, GO G T, PEI M, JUNG S, JEONG Y H, LEE W, PARK H L, KIM S W, YANG H, YANG C, LEE T W. Versatile neuromorphic electronics by modulating synaptic decay of single organic synaptic transistor: From artificial neural networks to neuro-prosthetics [J]. Nano Energy,2019,65:104035. [10] ZHAO Y, XIE Z, QIN C, QU Y, GENG Y, WANG L. Enhanced charge collection in polymer photovoltaic cells by using an ethanol-soluble conjugated polyfluorene as cathode buffer layer [J]. Solar Energy Materials and Solar Cells,2009,93(5):604-608. [11] 刘冠辰, 谢小银. 氯苯和邻二氯苯及其混合物作为溶剂对P3HT/PCBM异质结活性层光电转换效率的影响 [J]. 科学技术与工程,2016,16(1):13-16.LIU G C, XIE X Y. Solvent effects of chlorobenzene, ortho-dichlorobenzene and their mixture to performance of P3HT/PCBM-based bulk-heterojunction solar cells [J]. Science Technology and Engineering,2016,16(1):13-16. [12] CHANG J F, SUN B, BREIBY D W, NIELSEN M M, SÖLLING T I, GILES M, MCCULLOCH I, SIRRINGHAUS H. Enhanced mobility of poly(3-hexylthiophene) transistors by spin-coating from high-boiling-point solvents [J]. Chemistry of Materials,2004,16(23):4772-4776. [13] LEE K H, KANG M S, ZHANG S, GU Y, LODGE T P, FRISBIE C D. "Cut and stick" rubbery ion gels as high capacitance gate dielectrics [J]. Advanced Materials,2012,24(32):4457-4462. [14] PEUMANS P, YAKIMOV A, FORREST S R. Small molecular weight organic thin-film photodetectors and solar cells[J]. Journal of Applied Physics, 2003, 93(7): 3693-3723. [15] YANG S P, LI N, LI G, SHI J B, LI X W, FU G S. Effect of mixed solvents on P3HT: PCBM based solar cell [J]. Acta Physica Sinica,2013,62(1):014702. [16] MOULÉ A J, MEERHOLZ K. Controlling morphology in polymer-fullerene mixtures [J]. Advanced Materials,2008,20(2):240-245. [17] TSOI W C, JAMES D T, KIM J S, NICHOLSON P G, MURPHY C E, BRADLEY D D, NELSON J, KIM J S. The nature of in-plane skeleton raman modes of P3HT and their correlation to the degree of molecular order in P3HT: PCBM blend thin films [J]. Journal of the American Chemical Society,2011,133(25):9834-9843. [18] CHEN Q, HAN T, TANG M, ZHANG Z, ZHENG X, LIU G. Improving the recognition accuracy of memristive neural networks via homogenized analog type conductance quantization [J]. Micromachines (Basel),2020,11(4):427-436. -
下载:
点击查看大图
计量
- 文章访问数: 61
- HTML全文浏览量: 17
- PDF下载量: 17
- 被引次数: 0
