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Linearly programmable two-dimensional halide perovskite memristor arrays for neuromorphic computing

Nature Nanotechnology volume 20, pages 83–92 (2025)Cite this article

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Abstract

The exotic properties of three-dimensional halide perovskites, such as mixed ionic–electronic conductivity and feasible ion migration, have enabled them to challenge traditional memristive materials. However, the poor moisture stability and difficulty in controlling ion transport due to their polycrystalline nature have hindered their use as a neuromorphic hardware. Recently, two-dimensional (2D) halide perovskites have emerged as promising artificial synapses owing to their phase versatility, microstructural anisotropy in electrical and optoelectronic properties, and excellent moisture resistance. However, their asymmetrical and nonlinear conductance changes still limit the efficiency of training and accuracy of inference. Here we achieve highly linear and symmetrical conductance changes in Dion–Jacobson 2D perovskites. We further build a 7 × 7 crossbar array based on analogue perovskite synapses, achieving a high device yield, low variation with synaptic weight storing capability, multi-level analogue states with long retention, and moisture stability over 7 months. We explore the potential of such devices in large-scale image inference via simulations and show an accuracy within 0.08% of the theoretical limit. The excellent device performance is attributed to the elimination of gaps between inorganic layers, allowing the halide vacancies to migrate homogeneously regardless of grain boundaries. This was confirmed by first-principles calculations and experimental analysis.

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Fig. 1: Principle and demonstration of DJ-HP neuromorphic hardware.
Fig. 2: Materials characterization of DJ-phase 2D HPs.
Fig. 3: Synaptic plasticity of DJ-V-HP artificial synapses.
Fig. 4: Disclosing resistive switching mechanisms in DJ- and RP-phase HPs.
Fig. 5: Neuromorphic crossbar array for AI acceleration.

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Data availability

The data that support the conclusions of this study are available from the corresponding authors upon reasonable request. Source data are provided with this paper.

Code availability

The code that used for the software simulation for this study is available from the corresponding authors upon reasonable request.

Change history

  • 13 May 2025

    Since the version of the article initially published, the first sentence of the Acknowledgments section has been amended to “This research has been performed as a cooperation project (RS-2024-00421181) of the ‘Global C2H Research Center’ and supported by the Ministry of Science and ICT, Republic of Korea” in the HTML and PDF versions of the article.

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Acknowledgements

This research has been performed as a cooperation project (RS-2024-00421181) of the ‘Global C2H Research Center’ and supported by the Ministry of Science and ICT, Republic of Korea. This research was also supported by an NRF grant funded by the MSIT (2021R1A2B5B03001851, H.W.J.). J.J.Y. thanks the support of National Science Foundation under contract nos. 2023752 and 2036359. S.J.K. acknowledges the Basic Science Research Program through the NRF, funded by the Ministry of Education (2022R1A6A3A1306017211) and AI Institute at Seoul National University (AIIS). The Inter-University Semiconductor Research Center and Institute of Engineering Research at Seoul National University supported this work.

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Authors and Affiliations

  1. Department of Materials Science and Engineering, Research Institute of Advanced Materials, Seoul National University, Seoul, Republic of Korea

    Seung Ju Kim, In Hyuk Im, Ji Hyun Baek, Sungkyun Choi, Sung Hyuk Park, Da Eun Lee, Jae Young Kim & Ho Won Jang

  2. Ming Hsieh Department of Electrical and Computer Engineering, University of Southern California, Los Angeles, CA, USA

    Seung Ju Kim & J. Joshua Yang

  3. Department of Materials Science and Engineering, Institute of Green Manufacturing Technology, Korea University, Seoul, Republic of Korea

    Soo Young Kim

  4. School of Chemical Engineering, Center for Antibonding Regulated Crystals, Sungkyunkwan University, Suwon, Republic of Korea

    Nam-Gyu Park

  5. Department of Materials Science and Engineering, Pohang University of Science and Technology, Pohang, Republic of Korea

    Donghwa Lee

  6. Advanced Institute of Convergence Technology, Seoul National University, Suwon, Republic of Korea

    Ho Won Jang

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Contributions

S.J.K. D.L., J.J.Y. and H.W.J. conceived the project. S.J.K. fabricated and measured the devices and analysed the overall experimental results. I.H.I. helped with crossbar fabrication. J.H.B. helped with the deep learning process. S.C. carried out the TEM characterization. S.H.P. carried out the AFM characterization. D.E.L., J.Y.K., S.Y.K., N.-G.P. and J.J.Y. analysed the experimental results. D.L. conducted density first theory calculations. H.W.J. supervised the project. The manuscript was mainly written by S.J.K. D.L., J.J.Y. and H.W.J. All authors discussed the results and commented on the manuscript at all stages.

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Correspondence to Donghwa Lee, J. Joshua Yang or Ho Won Jang.

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Nature Nanotechnology thanks Kamal Asadi, Su-Ting Han and Peng Zhou for their contribution to the peer review of this work.

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Extended data

Extended Data Fig. 1 Research motivation and material design strategies of two-terminal halide perovskite memristors to achieve ideal analog switching behaviour.

(a) Moisture stability of 3D perovskites (that are vulnerable to moisture) is improved by reducing the dimension to 2D perovskites by adding hydrophobic large organic cations. (b) A schematic illustration of filamentary-type RP phase VCM memristor behaviour. Low crystalline (random-oriented) 2D perovskites cannot implement analog switching behaviour due to their poor ion mobility and inability to control ionic migration in the vertical direction. To demonstrate resistive switching behaviour, 2D perovskite nanocrystals were aligned perpendicular to the substrate via a pseudo-halide additive, which enables reliable synaptic behavior but shows asymmetric, nonlinear synaptic updates. (c) A schematic illustration of interfacial-type DJ phase VCM memristor behaviour. Interfacial-type VCM memristors show almost perfectly linear and symmetric conductance updates because their homogenous ion migration can gradually control the concentration of vacancies, resulting in gradual modulation of depletion layer width in the entire region.

Extended Data Fig. 2 Schematic illustration of crystal structure for comparing vacancy diffusion barrier energy through the large organic layer.

(a) lateral of the RP phase (BA2MA2Pb3I10, requiring 2.79 eV) and (b) lateral of DJ phase (BDAMA2Pb3I10, requiring 0.51 eV) two-dimensional halide perovskites. The distance between inorganic layers in the DJ phase (3.853 Å) is shorter than that of the RP phase. (7.244 Å) since the DJ phase perovskite has no van der Waals gap between inorganic layers.

Extended Data Fig. 3 Atomic force microscopy (AFM) and conductive atomic force microscopy (C-AFM) measurement with DJ phase perovskite films.

(a) A topological AFM mapping image of the DJ-V-HP/ITO glass structure with gold-coated tip. The tip moves 5 μm through the green dotted line to measure the roughness by distance. (b) C-AFM mapping images of the DJ-V-HP/ITO glass structure with tip biases of 0.05 V. The tip moves through the purple dotted line to measure the current versus the distance. (c) C-AFM mapping images of DJ-V-HP/ITO glass structure with tip biases of 1.5 V. The tip moves through the blue dotted line to measure the current versus the distance. It is noted that the topology mapping and the current mapping were acquired at the same location. (d) A schematic illustration of charged ion migration near the grain boundary in DJ-phase perovskites. The grain boundaries do not hinder the migration of charged ions across the grain, resulting in homogenous ion migration in all regions, regardless of grain boundaries.

Source data

Extended Data Fig. 4 Atomic force microscopy (AFM) and conductive atomic force microscopy (C-AFM) measurement with RP phase perovskite films.

(a) A topological AFM mapping image of the RP-V-HP/ITO glass structure. The tip moves 5 μm through the green dotted line to measure the roughness by distance. (b) C-AFM mapping images of the RP-V-HP/ITO glass structure with tip biases of 0.05 V. The tip moves through the purple dotted line to measure the current versus the distance. (c) C-AFM mapping images of the RP-V-HP/ITO glass structure with tip biases of 1.0 V. The tip moves through the blue dotted line to measure the current versus the distance. It is noted that the topology mapping and the current mapping were acquired at the same location. (d) A schematic illustration of charged ion migration near the grain boundary in RP-phase perovskites. The grain boundaries by the Van der Waals gap hinder the migration of charged ions across the grain, resulting in localized ion migration in certain grains.

Source data

Supplementary information

Supplementary Information

Supplementary Notes 1–9, Figs. 1–34, Tables 1 and 2, and References.

Source data

Source Data Fig. 2

Fig. 2a,b.

Source Data Fig. 3

Fig. 3a–f.

Source Data Fig. 4

Fig. 4c–f.

Source Data Fig. 5

Fig. 5a,b,d,g.

Source Data Extended Data Fig. 3

Extended Data Fig. 3a–c.

Source Data Extended Data Fig. 4

Extended Data Fig. 4a–c.

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Kim, S.J., Im, I.H., Baek, J.H. et al. Linearly programmable two-dimensional halide perovskite memristor arrays for neuromorphic computing. Nat. Nanotechnol. 20, 83–92 (2025). https://doi.org/10.1038/s41565-024-01790-3

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