Dielectric-Engineered Monolayer MoS2 Memtransistors for Brain-Inspired Computing with High Recognition Accuracy

Rajput, Manisha; Hwang, Sooyeon; Rahman, Atikur

doi:10.1021/acsami.5c11139

Dielectric-Engineered Monolayer MoS₂ Memtransistors for Brain-Inspired Computing with High Recognition Accuracy

Journal Article · Sun Sep 21 00:00:00 EDT 2025 · ACS Applied Materials & Interfaces

DOI:https://doi.org/10.1021/acsami.5c11139· OSTI ID:2998291

Rajput, Manisha ^[1]; ^[2]; ^[1]

Indian Institute of Science Education and Research (IISER), Pune (India)
Brookhaven National Laboratory (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)

Two-dimensional transition metal dichalcogenides (2D-TMDs)-based memtransistors have emerged as promising candidates for neuromorphic hardware due to their exceptional ability to emulate synaptic behavior. However, many existing 2D-TMDs memtransistors rely on polycrystalline channels with grain boundaries or defects introduced through postgrowth treatments, raising concerns about material integrity and the preservation of intrinsic properties. Here, in this work, we demonstrate a monocrystalline monolayer MoS₂ memtransistor fabricated on a silicon nitride (SiN_X) substrate, achieving a large resistive switching ratio of 10⁴, a dynamic range exceeding 90, along with highly linear and symmetric weight updates, minimal cycle-to-cycle variability, and low device-to-device variability. These attributes are critical for enabling high-performance neuromorphic hardware. Based on experimental data, we further show that these artificial synapses enable a recognition accuracy of more than 97% on the MNIST handwritten digits data set. Our findings present a straightforward approach to realizing 2D-TMDs memtransistors through dielectric engineering, offering a promising platform for next-generation neuromorphic computing systems.

View Accepted Manuscript (DOE)

Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

Grant/Contract Number:: SC0012704

OSTI ID:: 2998291

Report Number(s):: BNL--229044-2025-JAAM

Journal Information:: ACS Applied Materials & Interfaces, Journal Name: ACS Applied Materials & Interfaces Journal Issue: 39 Vol. 17; ISSN 1944-8244; ISSN 1944-8252

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

References (66)

From Bulk to Monolayer MoS2: Evolution of Raman Scattering Li, Hong; Zhang, Qing; Yap, Chin Chong Ray Advanced Functional Materials, Vol. 22, Issue 7 https://doi.org/10.1002/adfm.201102111	journal	January 2012
Artificial Synapses Based on Multiterminal Memtransistors for Neuromorphic Application Wang, Lin; Liao, Wugang; Wong, Swee Liang Advanced Functional Materials, Vol. 29, Issue 25 https://doi.org/10.1002/adfm.201901106	journal	April 2019
Dual‐Gated MoS ₂ Memtransistor Crossbar Array Lee, Hong‐Sub; Sangwan, Vinod K.; Rojas, William A. Gaviria Advanced Functional Materials, Vol. 30, Issue 45 https://doi.org/10.1002/adfm.202003683	journal	September 2020
2D Material Based Synaptic Devices for Neuromorphic Computing Cao, Guiming; Meng, Peng; Chen, Jiangang Advanced Functional Materials, Vol. 31, Issue 4 https://doi.org/10.1002/adfm.202005443	journal	October 2020
Non‐Volatile Electrolyte‐Gated Transistors Based on Graphdiyne/MoS₂ with Robust Stability for Low‐Power Neuromorphic Computing and Logic‐In‐Memory Yao, Bin‐Wei; Li, Jiaqiang; Chen, Xu‐Dong Advanced Functional Materials, Vol. 31, Issue 25 https://doi.org/10.1002/adfm.202100069	journal	April 2021
Low Power MoS ₂ /Nb ₂ O ₅ Memtransistor Device with Highly Reliable Heterosynaptic Plasticity Nam, Jae Hyeon; Oh, Seyoung; Jang, Hye Yeon Advanced Functional Materials, Vol. 31, Issue 40 https://doi.org/10.1002/adfm.202104174	journal	June 2021
Two‐Dimensional Memtransistors for Non‐Von Neumann Computing: Progress and Challenges Wali, Akshay; Das, Saptarshi Advanced Functional Materials, Vol. 34, Issue 15 https://doi.org/10.1002/adfm.202308129	journal	October 2023
Reconfigurable, Nonvolatile, Optoelectronic Synaptic Memtransistor Based on MoS₂/Te van der Waals Heterostructures Li, Yuan; Zhao, Min; Ma, Xiudong Advanced Functional Materials, Vol. 35, Issue 34 https://doi.org/10.1002/adfm.202423333	journal	March 2025
A MoS ₂ /PTCDA Hybrid Heterojunction Synapse with Efficient Photoelectric Dual Modulation and Versatility Wang, Shuiyuan; Chen, Chunsheng; Yu, Zhihao Advanced Materials, Vol. 31, Issue 3 https://doi.org/10.1002/adma.201806227	journal	September 2018
Memristors Based on 2D Materials as an Artificial Synapse for Neuromorphic Electronics Huh, Woong; Lee, Donghun; Lee, Chul‐Ho Advanced Materials, Vol. 32, Issue 51 https://doi.org/10.1002/adma.202002092	journal	September 2020
Progress and Challenges for Memtransistors in Neuromorphic Circuits and Systems Yan, Xiaodong; Qian, Justin H.; Sangwan, Vinod K. Advanced Materials, Vol. 34, Issue 48 https://doi.org/10.1002/adma.202108025	journal	February 2022
Photoinduced Multi‐Bit Nonvolatile Memory Based on a van der Waals Heterostructure with a 2D‐Perovskite Floating Gate Lai, Haojie; Zhou, Yang; Zhou, Huabin Advanced Materials, Vol. 34, Issue 19 https://doi.org/10.1002/adma.202110278	journal	April 2022
Heterosynaptic MoS₂ Memtransistors Emulating Biological Neuromodulation for Energy‐Efficient Neuromorphic Electronics Huh, Woong; Lee, Donghun; Jang, Seonghoon Advanced Materials, Vol. 35, Issue 24 https://doi.org/10.1002/adma.202211525	journal	April 2023
A Fully Printed Flexible MoS ₂ Memristive Artificial Synapse with Femtojoule Switching Energy Feng, Xuewei; Li, Yida; Wang, Lin Advanced Electronic Materials, Vol. 5, Issue 12 https://doi.org/10.1002/aelm.201900740	journal	September 2019
Programmable van‐der‐Waals heterostructure‐enabled optoelectronic synaptic floating‐gate transistors with ultra‐low energy consumption Sun, Yilin; Li, Mingjie; Ding, Yingtao InfoMat, Vol. 4, Issue 10 https://doi.org/10.1002/inf2.12317	journal	April 2022
Optical Identification of Single- and Few-Layer MoS2 Sheets Li, Hai; Lu, Gang; Yin, Zongyou Small, Vol. 8, Issue 5 https://doi.org/10.1002/smll.201101958	journal	January 2012
Optoelectronic Synaptic Memtransistor Based on 2D SnSe/MoS₂ van der Waals Heterostructure under UV–Ozone Treatment Yan, Yuling; Yu, Niannian; Yu, Ziyan Small Methods, Vol. 7, Issue 6 https://doi.org/10.1002/smtd.202201679	journal	March 2023
Characterization of SONOS oxynitride nonvolatile semiconductor memory devices Wrazien, Stephen J.; Zhao, Yijie; Krayer, Joel D. Solid-State Electronics, Vol. 47, Issue 5 https://doi.org/10.1016/S0038-1101(02)00448-3	journal	May 2003
Dielectric Engineered Two-Dimensional Neuromorphic Transistors Xiang, Du; Liu, Tao; Zhang, Xumeng Nano Letters, Vol. 21, Issue 8 https://doi.org/10.1021/acs.nanolett.1c00492	journal	April 2021
Reconfigurable MoS ₂ Memtransistors for Continuous Learning in Spiking Neural Networks Yuan, Jiangtan; Liu, Stephanie E.; Shylendra, Ahish Nano Letters, Vol. 21, Issue 15 https://doi.org/10.1021/acs.nanolett.1c00982	journal	July 2021
Atomristor: Nonvolatile Resistance Switching in Atomic Sheets of Transition Metal Dichalcogenides Ge, Ruijing; Wu, Xiaohan; Kim, Myungsoo Nano Letters, Vol. 18, Issue 1 https://doi.org/10.1021/acs.nanolett.7b04342	journal	December 2017
Vertical MoS ₂ Double-Layer Memristor with Electrochemical Metallization as an Atomic-Scale Synapse with Switching Thresholds Approaching 100 mV Xu, Renjing; Jang, Houk; Lee, Min-Hyun Nano Letters, Vol. 19, Issue 4 https://doi.org/10.1021/acs.nanolett.8b05140	journal	March 2019
In Situ Transport Measurements Reveal Source of Mobility Enhancement of MoS₂ and MoTe₂ during Dielectric Deposition Shang, Ju Ying; Moody, Michael J.; Chen, Jiazhen ACS Applied Electronic Materials, Vol. 2, Issue 5 https://doi.org/10.1021/acsaelm.0c00085	journal	April 2020
Demonstration of Nonvolatile Storage and Synaptic Functions in All-Two-Dimensional Floating-Gate Transistors Based on MoS₂ Channels Li, Wei; Li, Jiaying; Chen, Yuhua ACS Applied Electronic Materials, Vol. 5, Issue 8 https://doi.org/10.1021/acsaelm.3c00595	journal	July 2023
Energy-Efficient, Scalable Single-Layer MoS₂–Based Synaptic Field-Effect Transistors Kim, Jiman; Kim, Byeongju; Ma, Jiwon ACS Applied Electronic Materials, Vol. 7, Issue 14 https://doi.org/10.1021/acsaelm.5c00808	journal	June 2025
Double-Gate MoS ₂ Field-Effect Transistor with a Multilayer Graphene Floating Gate: A Versatile Device for Logic, Memory, and Synaptic Applications Rodder, Michael A.; Vasishta, Sudhanva; Dodabalapur, Ananth ACS Applied Materials & Interfaces, Vol. 12, Issue 30 https://doi.org/10.1021/acsami.0c08802	journal	July 2020
Highly Reproducible Heterosynaptic Plasticity Enabled by MoS₂/ZrO_2–x Heterostructure Memtransistor Jang, Hye Yeon; Kwon, Ojun; Nam, Jae Hyeon ACS Applied Materials & Interfaces, Vol. 14, Issue 46 https://doi.org/10.1021/acsami.2c15497	journal	November 2022
Artificial Synaptic Emulators Based on MoS₂ Flash Memory Devices with Double Floating Gates Yi, Sum-Gyun; Park, Myung Uk; Kim, Sung Hyun ACS Applied Materials & Interfaces, Vol. 10, Issue 37 https://doi.org/10.1021/acsami.8b10203	journal	August 2018
Electric and Light Dual-Gate Tunable MoS ₂ Memtransistor Yin, Siqi; Song, Cheng; Sun, Yiming ACS Applied Materials & Interfaces, Vol. 11, Issue 46 https://doi.org/10.1021/acsami.9b14259	journal	October 2019
Double-Floating-Gate van der Waals Transistor for High-Precision Synaptic Operations Cho, Hoyeon; Lee, Donghyun; Ko, Kyungmin ACS Nano, Vol. 17, Issue 8 https://doi.org/10.1021/acsnano.2c11538	journal	April 2023
Mimicking Neurotransmitter Release in Chemical Synapses via Hysteresis Engineering in MoS 2 Transistors Arnold, Andrew J.; Razavieh, Ali; Nasr, Joseph R. ACS Nano, Vol. 11, Issue 3 https://doi.org/10.1021/acsnano.7b00113	journal	February 2017
MoS ₂ Memristors Exhibiting Variable Switching Characteristics toward Biorealistic Synaptic Emulation Li, Da; Wu, Bin; Zhu, Xiaojian ACS Nano, Vol. 12, Issue 9 https://doi.org/10.1021/acsnano.8b03977	journal	September 2018
MoS ₂ Memtransistors Fabricated by Localized Helium Ion Beam Irradiation Jadwiszczak, Jakub; Keane, Darragh; Maguire, Pierce ACS Nano, Vol. 13, Issue 12 https://doi.org/10.1021/acsnano.9b07421	journal	December 2019
Artificial Optoelectronic Synapses Based on Ferroelectric Field-Effect Enabled 2D Transition Metal Dichalcogenide Memristive Transistors Luo, Zheng-Dong; Xia, Xue; Yang, Ming-Min ACS Nano, Vol. 14, Issue 1 https://doi.org/10.1021/acsnano.9b07687	journal	December 2019
Oxygen-Assisted Chemical Vapor Deposition Growth of Large Single-Crystal and High-Quality Monolayer MoS ₂ Chen, Wei; Zhao, Jing; Zhang, Jing Journal of the American Chemical Society, Vol. 137, Issue 50 https://doi.org/10.1021/jacs.5b10519	journal	December 2015
Nonvolatile Memory Cells Based on MoS ₂ /Graphene Heterostructures Bertolazzi, Simone; Krasnozhon, Daria; Kis, Andras ACS Nano, Vol. 7, Issue 4 https://doi.org/10.1021/nn3059136	journal	March 2013
Surface-Energy-Assisted Perfect Transfer of Centimeter-Scale Monolayer and Few-Layer MoS ₂ Films onto Arbitrary Substrates Gurarslan, Alper; Yu, Yifei; Su, Liqin ACS Nano, Vol. 8, Issue 11 https://doi.org/10.1021/nn5057673	journal	November 2014
Multi-terminal memtransistors from polycrystalline monolayer molybdenum disulfide Sangwan, Vinod K.; Lee, Hong-Sub; Bergeron, Hadallia Nature, Vol. 554, Issue 7693 https://doi.org/10.1038/nature25747	journal	February 2018
Layered memristive and memcapacitive switches for printable electronics Bessonov, Alexander A.; Kirikova, Marina N.; Petukhov, Dmitrii I. Nature Materials, Vol. 14, Issue 2 https://doi.org/10.1038/nmat4135	journal	November 2014
Wafer-scale solution-processed 2D material analog resistive memory array for memory-based computing Tang, Baoshan; Veluri, Hasita; Li, Yida Nature Communications, Vol. 13, Issue 1 https://doi.org/10.1038/s41467-022-30519-w	journal	June 2022
The gate injection-based field-effect synapse transistor with linear conductance update for online training Seo, Seokho; Kim, Beomjin; Kim, Donghoon Nature Communications, Vol. 13, Issue 1 https://doi.org/10.1038/s41467-022-34178-9	journal	October 2022
Programmable nonlinear optical neuromorphic computing with bare 2D material MoS2 Tong, Lei; Bi, Yali; Wang, Yilun Nature Communications, Vol. 15, Issue 1 https://doi.org/10.1038/s41467-024-54776-z	journal	November 2024
SiGe epitaxial memory for neuromorphic computing with reproducible high performance based on engineered dislocations Choi, Shinhyun; Tan, Scott H.; Li, Zefan Nature Materials, Vol. 17, Issue 4 https://doi.org/10.1038/s41563-017-0001-5	journal	January 2018
Observation of single-defect memristor in an MoS2 atomic sheet Hus, Saban M.; Ge, Ruijing; Chen, Po-An Nature Nanotechnology, Vol. 16, Issue 1 https://doi.org/10.1038/s41565-020-00789-w	journal	November 2020
Two-dimensional materials for next-generation computing technologies Liu, Chunsen; Chen, Huawei; Wang, Shuiyuan Nature Nanotechnology, Vol. 15, Issue 7 https://doi.org/10.1038/s41565-020-0724-3	journal	July 2020
Engineering MoSe2/MoS2 heterojunction traps in 2D transistors for multilevel memory, multiscale display, and synaptic functions Jeong, Yeonsu; Lee, Han Joo; Park, Junkyu npj 2D Materials and Applications, Vol. 6, Issue 1 https://doi.org/10.1038/s41699-022-00295-8	journal	March 2022
Fully memristive neural networks for pattern classification with unsupervised learning Wang, Zhongrui; Joshi, Saumil; Savel’ev, Sergey Nature Electronics, Vol. 1, Issue 2 https://doi.org/10.1038/s41928-018-0023-2	journal	February 2018
Electronic synapses made of layered two-dimensional materials Shi, Yuanyuan; Liang, Xianhu; Yuan, Bin Nature Electronics, Vol. 1, Issue 8 https://doi.org/10.1038/s41928-018-0118-9	journal	August 2018
Defect-engineered monolayer MoS2 with enhanced memristive and synaptic functionality for neuromorphic computing Rajput, Manisha; Mallik, Sameer Kumar; Chatterjee, Sagnik Communications Materials, Vol. 5, Issue 1 https://doi.org/10.1038/s43246-024-00632-y	journal	September 2024
A high linearity and energy-efficient artificial synaptic device based on scalable synthesized MoS₂ Zhao, Yuxin; Jin, Yuanhao; Wang, Xing Journal of Materials Chemistry C, Vol. 11, Issue 17 https://doi.org/10.1039/D3TC00438D	journal	January 2023
Nonvolatile polycrystalline silicon thin film transistor memory using silicon-rich silicon nitride as charge storage layer Pei, Z.; Chung, A.; Hwang, H. L. Applied Physics Letters, Vol. 90, Issue 22 https://doi.org/10.1063/1.2745265	journal	May 2007
Nature of traps responsible for the memory effect in silicon nitride Gritsenko, V. A.; Perevalov, T. V.; Orlov, O. M. Applied Physics Letters, Vol. 109, Issue 6 https://doi.org/10.1063/1.4959830	journal	August 2016
Reliability of analog resistive switching memory for neuromorphic computing Zhao, Meiran; Gao, Bin; Tang, Jianshi Applied Physics Reviews, Vol. 7, Issue 1 https://doi.org/10.1063/1.5124915	journal	March 2020
Memtransistor-like operation of devices made by graphene/h-BN/MoS2 van der Waals heterostructure Chien, Shih-Po; Liang, Bor-Wei; Chang, Wen-Hao Applied Physics Letters, Vol. 123, Issue 14 https://doi.org/10.1063/5.0165606	journal	October 2023
Roadmap to neuromorphic computing with emerging technologies Mehonic, Adnan; Ielmini, Daniele; Roy, Kaushik APL Materials, Vol. 12, Issue 10 https://doi.org/10.1063/5.0179424	journal	October 2024
Optimized pulsed write schemes improve linearity and write speed for low-power organic neuromorphic devices Keene, Scott T.; Melianas, Armantas; Fuller, Elliot J. Journal of Physics D: Applied Physics, Vol. 51, Issue 22 https://doi.org/10.1088/1361-6463/aabe70	journal	May 2018
Improvement of analogue switching characteristics of MoS ₂ memristors through plasma treatment Li, Da; Ryu, Byunghoon; Yoon, JeongSeop Journal of Physics D: Applied Physics, Vol. 53, Issue 13 https://doi.org/10.1088/1361-6463/ab6572	journal	January 2020
Effect of conductance linearity and multi-level cell characteristics of TaO_x-based synapse device on pattern recognition accuracy of neuromorphic system Sung, Changhyuck; Lim, Seokjae; Kim, Hyungjun Nanotechnology, Vol. 29, Issue 11 https://doi.org/10.1088/1361-6528/aaa733	journal	February 2018
Mitigating Asymmetric Nonlinear Weight Update Effects in Hardware Neural Network Based on Analog Resistive Synapse Chang, Chih-Cheng; Chen, Pin-Chun; Chou, Teyuh IEEE Journal on Emerging and Selected Topics in Circuits and Systems, Vol. 8, Issue 1 https://doi.org/10.1109/JETCAS.2017.2771529	journal	March 2018
Improved Synaptic Behavior Under Identical Pulses Using AlO x /HfO 2 Bilayer RRAM Array for Neuromorphic Systems Woo, Jiyong; Moon, Kibong; Song, Jeonghwan IEEE Electron Device Letters, Vol. 37, Issue 8 https://doi.org/10.1109/LED.2016.2582859	journal	August 2016
High-Performance Floating Gate Heterostructure With WSe₂-MoS₂ Diode Channel for Neural Synapse Su, Zijia; Cheng, Hengxiao; Sun, Xiyu IEEE Electron Device Letters, Vol. 44, Issue 7 https://doi.org/10.1109/LED.2023.3278454	journal	July 2023
Analyzing the Effect of High-k Dielectric-Mediated Doping on Contact Resistance in Top-Gated Monolayer MoS₂ Transistors Alharbi, Abdullah; Shahrjerdi, Davood IEEE Transactions on Electron Devices, Vol. 65, Issue 10 https://doi.org/10.1109/TED.2018.2866772	journal	October 2018
A million spiking-neuron integrated circuit with a scalable communication network and interface Merolla, P. A.; Arthur, J. V.; Alvarez-Icaza, R. Science, Vol. 345, Issue 6197 https://doi.org/10.1126/science.1254642	journal	August 2014
Memfractance: A Mathematical Paradigm for Circuit Elements with Memory Abdelouahab, Mohammed-Salah; Lozi, René; Chua, Leon International Journal of Bifurcation and Chaos, Vol. 24, Issue 09 https://doi.org/10.1142/S0218127414300237	journal	September 2014
CMOS design near the limit of scaling Taur, Y. IBM Journal of Research and Development, Vol. 46, Issue 2.3 https://doi.org/10.1147/rd.462.0213	journal	March 2002
Training Deep Convolutional Neural Networks with Resistive Cross-Point Devices Gokmen, Tayfun; Onen, Murat; Haensch, Wilfried Frontiers in Neuroscience, Vol. 11 https://doi.org/10.3389/fnins.2017.00538	journal	October 2017

Similar Records

Defect-engineered monolayer MoS₂ with enhanced memristive and synaptic functionality for neuromorphic computing

Journal Article · Sun Sep 15 20:00:00 EDT 2024 · Communications Materials · OSTI ID:2448247

Influence of surface adsorption on MoS₂ memtransistor switching kinetics

Journal Article · Tue May 30 00:00:00 EDT 2023 · Applied Physics Letters · OSTI ID:2311629

Progress and Challenges for Memtransistors in Neuromorphic Circuits and Systems

Journal Article · Mon Nov 22 23:00:00 EST 2021 · Advanced Materials · OSTI ID:2424312

Related Subjects

2D TMDs
75 CONDENSED MATTER PHYSICS
SUPERCONDUCTIVITY AND SUPERFLUIDITY
dielectric-engineering
memristor
memtransistor
neuromorphic computing
synaptic plasticity

Dielectric-Engineered Monolayer MoS2 Memtransistors for Brain-Inspired Computing with High Recognition Accuracy

Citation Formats

References (66)

Similar Records

Related Subjects

Dielectric-Engineered Monolayer MoS₂ Memtransistors for Brain-Inspired Computing with High Recognition Accuracy