Abstract
Memristive devices can offer dynamic behaviour, analogue programmability, and scaling and integration capabilities. As a result, they are of potential use in the development of information processing and storage devices for both conventional and unconventional computing paradigms. Their memristive switching processes originate mainly from the modulation of the number and position of structural defects or compositional impurities—what are commonly referred to as imperfections. While the underlying mechanisms and potential applications of memristors based on traditional bulk materials have been extensively studied, memristors based on van der Waals materials have only been considered more recently. Here we examine imperfection-enabled memristive switching in van der Waals materials. We explore how imperfections—together with the inherent physicochemical properties of the van der Waals materials—create different switching mechanisms, and thus provide a range of opportunities to engineer switching behaviour in memristive devices. We also discuss the challenges involved in terms of material selection, mechanism investigation and switching uniformity control, and consider the potential of van der Waals memristors in system-level implementations of efficient computing technologies.
This is a preview of subscription content, access via your institution
Access options
Access Nature and 54 other Nature Portfolio journals
Get Nature+, our best-value online-access subscription
$29.99 / 30 days
cancel any time
Subscribe to this journal
Receive 12 digital issues and online access to articles
$119.00 per year
only $9.92 per issue
Buy this article
- Purchase on Springer Link
- Instant access to full article PDF
Prices may be subject to local taxes which are calculated during checkout
Similar content being viewed by others
References
Lanza, M. et al. Memristive technologies for data storage, computation, encryption, and radio-frequency communication. Science 376, 1066 (2022).
Zhou, F. et al. Optoelectronic resistive random access memory for neuromorphic vision sensors. Nat. Nanotechnol. 14, 776–782 (2019).
Rao, M. et al. Thousands of conductance levels in memristors integrated on CMOS. Nature 615, 823–829 (2023).
Yang, J. J. et al. Memristive switching mechanism for metal/oxide/metal nanodevices. Nat. Nanotechnol. 3, 429–433 (2008).
Li, C. et al. Direct observations of nanofilament evolution in switching processes in HfO2-based resistive random access memory by in situ TEM studies. Adv. Mater. 29, 1602976 (2017).
Yuan, F. et al. Real-time observation of the electrode-size-dependent evolution dynamics of the conducting filaments in a SiO2 layer. ACS Nano 11, 4097–4104 (2017).
Yang, J. J., Strukov, D. B. & Stewart, D. R. Memristive devices for computing. Nat. Nanotechnol. 8, 13–24 (2013).
Chen, Y.-S. et al. An ultrathin forming-free HfOx resistance memory with excellent electrical performance. IEEE Electron Device Lett. 31, 1473–1475 (2010).
Panja, R., Roy, S., Jana, D. & Maikap, S. Impact of device size and thickness of Al2O3 film on the Cu pillar and resistive switching characteristics for 3D cross-point memory application. Nanoscale Res. Lett. 9, 692 (2014).
Chen, A. Area and thickness scaling of forming voltage of resistive switching memories. IEEE Electron Device Lett. 35, 57–59 (2014).
Liu, S. et al. Eliminating negative-SET behavior by suppressing nanofilament overgrowth in cation-based memory. Adv. Mater. 28, 10623–10629 (2016).
Zhao, H. et al. Atomically thin femtojoule memristive device. Adv. Mater. 29, 1703232 (2017). This paper exploited the atomic level uniformity of vdW materials and demonstrated a memristive device with sub-nanometre medium thickness and low power consumption.
Shi, Y. et al. Electronic synapses made of layered two-dimensional materials. Nat. Electron. 1, 458–465 (2018).
Chen, S. et al. Wafer-scale integration of two-dimensional materials in high-density memristive crossbar arrays for artificial neural networks. Nat. Electron. 3, 638–645 (2020).
Wang, X. et al. Grain-boundary engineering of monolayer MoS2 for energy-efficient lateral synaptic devices. Adv. Mater. 33, 2102435 (2021).
Sangwan, V. K. et al. Gate-tunable memristive phenomena mediated by grain boundaries in single-layer MoS2. Nat. Nanotechnol. 10, 403–406 (2015).
Liu, X. W. et al. Temperature-sensitive spatial distribution of defects in PdSe2 flakes. Phys. Rev. Mater. 5, L041001 (2021).
Lin, Y. C., Dumcenco, D. O., Huang, Y. S. & Suenaga, K. Atomic mechanism of the semiconducting-to-metallic phase transition in single-layered MoS2. Nat. Nanotechnol. 9, 391–396 (2014).
Hus, S. M. et al. Observation of single-defect memristor in an MoS2 atomic sheet. Nat. Nanotechnol. 16, 58–62 (2021). This work revealed the switching process in a single-vacancy monolayer MoS2 memristor and its potential in realizing the smallest-footprint devices.
Sangwan, V. K. et al. Multi-terminal memtransistors from polycrystalline monolayer molybdenum disulfide. Nature 554, 500–504 (2018). This study demonstrated the gate-tunable heterosynaptic functionality in lateral MoS2 memristors.
Azizi, A. et al. Dislocation motion and grain boundary migration in two-dimensional tungsten disulphide. Nat. Commun. 5, 4867 (2014).
Zhu, X., Li, D., Liang, X. & Lu, W. D. Ionic modulation and ionic coupling effects in MoS2 devices for neuromorphic computing. Nat. Mater. 18, 141–148 (2019). This paper reported a phase-transition-enabled memristor based on field-driven ionic modulation.
Fang, Z. et al. Temperature instability of resistive switching on HfOx-based RRAM devices. IEEE Electron Device Lett. 31, 476–478 (2010).
Wang, M. et al. Robust memristors based on layered two-dimensional materials. Nat. Electron. 1, 130–136 (2018). This study reported a robust vdW memristive device with a high operating temperature enabled by the oxidisation of MoS2 flakes.
He, Y. et al. Engineering grain boundaries at the 2D limit for the hydrogen evolution reaction. Nat. Commun. 11, 57 (2020).
Zhou, W. et al. Intrinsic structural defects in monolayer molybdenum disulfide. Nano Lett. 13, 2615–2622 (2013).
Zou, X. & Yakobson, B. Defects in Two-Dimensional Materials. In Avouris, P., Heinz, T. & Low, T. (Eds.), 2D Materials: Properties and Devices (pp. 359-378) (2017) Cambridge: Cambridge University Press
Ma, J., Alfè, D., Michaelides, A. & Wang, E. Stone–Wales defects in graphene and other planar sp2-bonded materials. Phys. Rev. B 80, 033407 (2009).
van der Zande, A. M. et al. Grains and grain boundaries in highly crystalline monolayer molybdenum disulphide. Nat. Mater. 12, 554–561 (2013).
Lahiri, J., Lin, Y., Bozkurt, P., Oleynik, I. I. & Batzill, M. An extended defect in graphene as a metallic wire. Nat. Nanotechnol. 5, 326–329 (2010).
Li, Y., Yan, H., Xu, B., Zhen, L. & Xu, C. Y. Electrochemical intercalation in atomically thin van der Waals materials for structural phase transition and device applications. Adv. Mater. 33, 2000581 (2021).
Su, C. et al. Engineering single-atom dynamics with electron irradiation. Sci. Adv. 5, eaav2252 (2019).
Tosun, M. et al. Air-stable n-doping of WSe2 by anion vacancy formation with mild plasma treatment. ACS Nano 10, 6853–6860 (2016).
Li, J. The mechanics and physics of defect nucleation. MRS Bull. 32, 151–159 (2011).
Li, W., Qian, X. & Li, J. Phase transitions in 2D materials. Nat. Rev. Mater. 6, 829–846 (2021).
Duerloo, K.-A. & Reed, E. J. Structural phase transitions by design in monolayer alloys. ACS Nano 10, 289–297 (2016).
Bessonov, A. A. et al. Layered memristive and memcapacitive switches for printable electronics. Nat. Mater. 14, 199–204 (2015).
Pam, M. E. et al. Interface-modulated resistive switching in Mo-irradiated ReS2 for neuromorphic computing. Adv. Mater. 34, 2202722 (2022).
Gong, Y. et al. Spatially controlled doping of two-dimensional SnS2 through intercalation for electronics. Nat. Nanotechnol. 13, 294–299 (2018).
Li, M. et al. High mobilities in layered InSe transistors with indium-encapsulation-induced surface charge doping. Adv. Mater. 30, 1803690 (2018).
Shen, Y. et al. Variability and yield in h-BN-based memristive circuits: the role of each type of defect. Adv. Mater. 33, 2103656 (2021).
Garaj, S. et al. Graphene as a subnanometre trans-electrode membrane. Nature 467, 190–193 (2010).
Lee, J., Du, C., Sun, K., Kioupakis, E. & Lu, W. D. Tuning ionic transport in memristive devices by graphene with engineered nanopores. ACS Nano 10, 3571–3579 (2016).
Ge, R. et al. Atomristor: nonvolatile resistance switching in atomic sheets of transition metal dichalcogenides. Nano Lett. 18, 434–441 (2018).
Sun, L. et al. Self-selective van der Waals heterostructures for large scale memory array. Nat. Commun. 10, 3161 (2019).
Wu, X. et al. Thinnest nonvolatile memory based on monolayer h-BN. Adv. Mater. 31, 1806790 (2019).
Ge, R. et al. A library of atomically thin 2D materials featuring the conductive-point resistive switching phenomenon. Adv. Mater. 33, 2007792 (2020).
Li, Y. S. et al. Anomalous resistive switching in memristors based on two-dimensional palladium diselenide using heterophase grain boundaries. Nat. Electron. 4, 348–356 (2021).
Zhang, D., Yeh, C.-H., Cao, W. & Banerjee, K. 0.5T0.5R—an ultracompact RRAM cell uniquely enabled by van der Waals heterostructures. IEEE Trans. Electron Devices 68, 2033–2040 (2021).
Zhao, X. et al. Confining cation injection to enhance CBRAM performance by nanopore graphene layer. Small 13, 1603948 (2017). This work employed nanoporous graphene to regulate the morphology and spatial distribution of conductive channels in metal-oxide memristors.
Yan, Y., Sun, B. & Ma, D. Resistive switching memory characteristics of single MoSe2 nanorods. Chem. Phys. Lett. 638, 103–107 (2015).
Pan, C. et al. Coexistence of grain-boundaries-assisted bipolar and threshold resistive switching in multilayer hexagonal boron nitride. Adv. Funct. Mater. 27, 1604811 (2017).
Xu, R. et al. Vertical MoS2 double-layer memristor with electrochemical metallization as an atomic-scale synapse with switching thresholds approaching 100 mV. Nano Lett. 19, 2411–2417 (2019).
Frey, N. C., Akinwande, D., Jariwala, D. & Shenoy, V. B. Machine learning-enabled design of point defects in 2D materials for quantum and neuromorphic information processing. ACS Nano 14, 13406–13417 (2020).
Son, D. et al. Colloidal synthesis of uniform-sized molybdenum disulfide nanosheets for wafer-scale flexible nonvolatile memory. Adv. Mater. 28, 9326–9332 (2016).
Yan, X. et al. Vacancy-induced synaptic behavior in 2D WS2 nanosheet-based memristor for low-power neuromorphic computing. Small 15, 1901423 (2019).
Feng, X. et al. Self-selective multi-terminal memtransistor crossbar array for in-memory computing. ACS Nano 15, 1764–1774 (2021).
Song, D.-X., Ma, W.-G. & Zhang, X. Correlated migration of ions in a 2D heterostructure anode: guaranteeing a low barrier for a high site occupancy. J. Mater. Chem. A 8, 17463–17470 (2020).
Wang, L. et al. Artificial synapses based on multiterminal memtransistors for neuromorphic application. Adv. Funct. Mater. 29, 1901106 (2019).
Wang, Y. et al. High on/off ratio black phosphorus based memristor with ultra-thin phosphorus oxide layer. Appl. Phys. Lett. 115, 193503 (2019).
Liu, L. et al. Low-power memristive logic device enabled by controllable oxidation of 2D HfSe2 for in-memory computing. Adv. Sci. 8, 2005038 (2021).
Huh, W. et al. Synaptic barristor based on phase-engineered 2D heterostructures. Adv. Mater. 30, 1801447 (2018).
Yamamoto, M. et al. Self-limiting layer-by-layer oxidation of atomically thin WSe2. Nano Lett. 15, 2067–2073 (2015).
Liu, Y. et al. Thermal oxidation of WSe2 nanosheets adhered on SiO2/Si substrates. Nano Lett. 15, 4979–4984 (2015).
Yang, F. S. et al. Oxidation-boosted charge trapping in ultra-sensitive van der Waals materials for artificial synaptic features. Nat. Commun. 11, 2972 (2020).
Mleczko, M. J. et al. HfSe2 and ZrSe2: two-dimensional semiconductors with native high-kappa oxides. Sci. Adv. 3, 1700481 (2017).
Duerloo, K. A., Li, Y. & Reed, E. J. Structural phase transitions in two-dimensional Mo- and W-dichalcogenide monolayers. Nat. Commun. 5, 4214 (2014).
Yang, H., Kim, S. W., Chhowalla, M. & Lee, Y. H. Structural and quantum-state phase transitions in van der Waals layered materials. Nat. Phys. 13, 931–937 (2017). This paper critically examined the phase transition physics in vdW materials and highlighted the perspective applications of vdW electronics.
Wang, Y. et al. Structural phase transition in monolayer MoTe2 driven by electrostatic doping. Nature 550, 487–491 (2017).
Rao, F. et al. Reducing the stochasticity of crystal nucleation to enable subnanosecond memory writing. Science 358, 1423–1427 (2017).
Zhang, F. et al. An ultra-fast multi-level MoTe2-based RRAM. In 2018 IEEE International Electron Devices Meeting (IEDM) 22.7.1–22.7.4 (IEEE, 2019).
Zhang, F. et al. Electric-field induced structural transition in vertical MoTe2- and Mo1−xWTe2-based resistive memories. Nat. Mater. 18, 55–61 (2019).
Cheng, P., Sun, K. & Hu, Y. H. Memristive behavior and ideal memristor of 1T phase MoS2 nanosheets. Nano Lett. 16, 572–576 (2016).
Jin, Q., Liu, N., Chen, B. & Mei, D. Mechanisms of semiconducting 2H to metallic 1T phase transition in two-dimensional MoS2 nanosheets. J. Phys. Chem. C 122, 28215–28224 (2018).
Han, S. T. et al. Black phosphorus quantum dots with tunable memory properties and multilevel resistive switching characteristics. Adv. Sci. 4, 1600435 (2017).
Yao, J. et al. Resistive switching in nanogap systems on SiO2 substrates. Small 5, 2910–2915 (2009).
Hong, S. K., Kim, J. E., Kim, S. O., Choi, S.-Y. & Cho, B. J. Flexible resistive switching memory device based on graphene oxide. IEEE Electron Device Lett. 31, 1005–1007 (2010).
Wang, Z. et al. Resistive switching materials for information processing. Nat. Rev. Mater. 5, 173–195 (2020).
Jo, S. H. et al. Nanoscale memristor device as synapse in neuromorphic systems. Nano Lett. 10, 1297–1301 (2010).
Ma, C. et al. Intelligent infrared sensing enabled by tunable moiré quantum geometry. Nature 604, 266–272 (2022).
Feng, X. et al. A fully printed flexible MoS2 memristive artificial synapse with femtojoule switching energy. Adv. Electron. Mater. 5, 1900740 (2019).
Li, Y., Long, S., Liu, Q., Lv, H. & Liu, M. Resistive switching performance improvement via modulating nanoscale conductive filament, involving the application of two-dimensional layered materials. Small 13, 1604306 (2017).
Li, X. et al. Power-efficient neural network with artificial dendrites. Nat. Nanotechnol. 15, 776–782 (2020).
Kalita, H. et al. Artificial neuron using vertical MoS2/graphene threshold switching memristors. Sci. Rep. 9, 53 (2019).
Liu, H. et al. A tantalum disulfide charge-density-wave stochastic artificial neuron for emulating neural statistical properties. Nano Lett. 21, 3465–3472 (2021).
Pi, S., Ghadiri-Sadrabadi, M., Bardin, J. C. & Xia, Q. F. Nanoscale memristive radiofrequency switches. Nat. Commun. 6, 7519 (2015).
Kim, M. et al. Analogue switches made from boron nitride monolayers for application in 5G and terahertz communication systems. Nat. Electron. 3, 479–485 (2020). This study reported the monolayer h-BN memristor and its application in radiofrequency switches.
Kim, M. et al. Monolayer molybdenum disulfide switches for 6G communication systems. Nat. Electron. 5, 367–373 (2022).
Lanza, M., Smets, Q., Huyghebaert, C. & Li, L.-J. Yield, variability, reliability, and stability of two-dimensional materials based solid-state electronic devices. Nat. Commun. 11, 5689 (2020).
Choi, S. et al. SiGe epitaxial memory for neuromorphic computing with reproducible high performance based on engineered dislocations. Nat. Mater. 17, 335–340 (2018). This work demonstrated SiGe epitaxial memristors with engineered grain boundary distribution and provided inspiration for variation control of vdW memristors.
Chen, T. A. et al. Wafer-scale single-crystal hexagonal boron nitride monolayers on Cu(111). Nature 579, 219–223 (2020).
Wang, Z. R. et al. Memristors with diffusive dynamics as synaptic emulators for neuromorphic computing. Nat. Mater. 16, 101–108 (2017).
Sun, L., Banhart, F. & Warner, J. Two-dimensional materials under electron irradiation. MRS Bull. 40, 29–37 (2015).
Rollings, R. C., Kuan, A. T. & Golovchenko, J. A. Ion selectivity of graphene nanopores. Nat. Commun. 7, 11408 (2016).
Zhao, X. et al. Breaking the current-retention dilemma in cation-based resistive switching devices utilizing graphene with controlled defects. Adv. Mater. 30, 1705193 (2018).
Ambrogio, S. et al. Equivalent-accuracy accelerated neural-network training using analogue memory. Nature 558, 60–67 (2018).
Hinton, H. et al. A 200 × 256 image sensor heterogeneously integrating a 2D nanomaterial-based photo-FET array and CMOS time-to-digital converters. In 2022 IEEE International Solid-State Circuits Conference (ISSCC) 12.2.1–12.2.3 (IEEE, 2022). This paper provided the fabrication contexts of vdW device and CMOS integrated circuits.
Zhu, K. et al. Hybrid 2D/CMOS microchips for memristive applications. Nature 618, 57–62 (2023).
Zhao, Y. et al. Large-area transfer of two-dimensional materials free of cracks, contamination and wrinkles via controllable conformal contact. Nat. Commun. 13, 4409 (2022).
Pi, S. et al. Memristor crossbar arrays with 6-nm half-pitch and 2-nm critical dimension. Nat. Nanotechnol. 14, 35–39 (2019).
Jiang, J., Parto, K., Cao, W. & Banerjee, K. Ultimate monolithic-3D integration with 2D materials: rationale, prospects, and challenges. IEEE J. Electron Devices Soc. 7, 878–887 (2019).
Luo, Q. et al. A highly CMOS compatible hafnia-based ferroelectric diode. Nat. Commun. 11, 1391 (2020).
IEEE International Roadmap for Devices and Systems (IRDS™) 2022 Edition https://irds.ieee.org/editions/2022 (2022).
Acknowledgements
We thank M.-Y. Tsai for constructive suggestions on the figure optimization. M.L. and Y.-F.L. acknowledge support from the Taiwan Ministry of Science and Technology (grants MOST 109-2112-M-005-013-MY3 and 110-2881-M-005-512-MY2). H.L. and H.W. acknowledge the support of the Army Research Office (grant W911NF1810268) and National Science Foundation (grants 2036359 and 1653870). This work was partially supported by the Air Force Office of Scientific Research (AFOSR) through the Multidisciplinary University Research Initiative (MURI) programme under contract FA9550-19-1-0213 and the United States Air Force Research Laboratory (AFRL) under grants FA8750-18-2-0122 and FA8650-21-C-5405. This work was also partially supported by the National Science Foundation under contract 2023752. The opinions, findings and conclusions or recommendations expressed in this material are those of the authors and do not necessarily reflect the views of AFRL.
Author information
Authors and Affiliations
Contributions
J.J.Y., Y.-F.L. and H.W. conceived the concepts and perspectives. M.L., H.L. and R.Z. worked on literature analysis and data collection. M.L., H.L. and J.J.Y. co-wrote the manuscript. All authors contributed to the discussion of content and reviewed and edited the manuscript. J.J.Y. supervised the project at all stages.
Corresponding authors
Ethics declarations
Competing interests
The authors declare no competing interests.
Peer review
Peer review information
Nature Electronics thanks Jun Lou, Kah-Wee Ang and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.
Additional information
Publisher’s note Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
Supplementary information
Supplementary Information
Supplementary Figs. 1–3 and Tables 1–4.
Rights and permissions
Springer Nature or its licensor (e.g. a society or other partner) holds exclusive rights to this article under a publishing agreement with the author(s) or other rightsholder(s); author self-archiving of the accepted manuscript version of this article is solely governed by the terms of such publishing agreement and applicable law.
About this article
Cite this article
Li, M., Liu, H., Zhao, R. et al. Imperfection-enabled memristive switching in van der Waals materials. Nat Electron 6, 491–505 (2023). https://doi.org/10.1038/s41928-023-00984-2
Received:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1038/s41928-023-00984-2
This article is cited by
-
Modulating p-type doping of two dimensional material palladium diselenide
Nano Research (2024)
-
Monolithic 3D integration of 2D materials-based electronics towards ultimate edge computing solutions
Nature Materials (2023)