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Anomalous resistive switching in memristors based on two-dimensional palladium diselenide using heterophase grain boundaries

Abstract

The implementation of memristive synapses in neuromorphic computing is hindered by the limited reproducibility and high energy consumption of the switching behaviour of the devices. Typical filament-type memristors suffer, in particular, from temporal and spatial variation in the set voltage and resistance states due to stochastic filament formation. Here, we report memristors based on two-dimensional pentagonal palladium diselenide (PdSe2) that can exhibit anomalous resistive switching behaviour with two interchangeable reset modes: total reset and quasi-reset. Heterophase grain boundaries are formed in the PdSe2 via local phase transitions induced by electron-beam irradiation, which leads to residual filaments along the grain boundaries that can guide the formation of conductive filaments. When operated in the quasi-reset mode, the memristors show a sixfold improvement in switching variation compared with devices operating in the total-reset mode, as well as a low set voltage (0.6 V), long retention times and programmable multilevel resistance states. We also show that the devices can emulate synaptic plasticity and that multipattern memorization can be implemented using a crossbar array architecture.

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Fig. 1: Ti/e-beam-irradiated PdSe2/Au memristor.
Fig. 2: Heterophase grain boundary formation by e-beam irradiation.
Fig. 3: Interchangeable reset mode in the e-beam-irradiated PdSe2 memristor.
Fig. 4: Reliable and multilevel RS in quasi-reset mode.
Fig. 5: E-beam-irradiated PdSe2 memristor in the quasi-reset mode for neuromorphic computing.
Fig. 6: E-beam-irradiated PdSe2 memristor in crossbar array architecture for pattern memorization.

Data availability

The data that support the plots within this article and other findings of this study are available from the corresponding author upon reasonable request.

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Acknowledgements

This work is supported by A*STAR Science and Engineering Research Council (no. A2083c0061), and by the National Research Foundation, Prime Minister’s Office, Singapore, under its Competitive Research Programme (NRF-CRP24-2020-050). We thank A. V.-Y. Thean, Y. Li, X. Feng and X. Gong in the Department of Electrical and Computer Engineering, and K. P. Loh and L. Wang in the Department of Chemistry, National University of Singapore, for valuable help in device measurements.

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This project was supervised and directed by K.-W.A. Y.L. and K.-W.A. conceived this work. Y.L. and K.-W.A. designed the experiments. Y.L., S.L. and B.L. performed the device fabrication. Y.L. and S.L. conducted the electrical measurements. Y.L. and L.C. performed the material characterization. L.L. and M.B. performed the STEM-ADF imaging. All authors contributed to the discussion and analysis of results. Y.L. and K.-W.A. wrote the manuscript.

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Correspondence to Kah-Wee Ang.

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Supplementary Figs. 1–21, Discussion and Tables 1 and 2.

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Li, Y., Loh, L., Li, S. et al. Anomalous resistive switching in memristors based on two-dimensional palladium diselenide using heterophase grain boundaries. Nat Electron 4, 348–356 (2021). https://doi.org/10.1038/s41928-021-00573-1

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