Molecular Engineering of Interlayer Spacings in 2D Dion-Jacobson Perovskites for High-Fidelity Neuromorphic Computing.

Liu, Binglin; Lee, Hyeon-Ji; Park, Sunbeom; Kim, Hee A; Yang, Qingyu; Liang, Jian; Gu, Guangjie; Jiang, Bowen et al. · ACS Nano · 2026

basic_science · Level V

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Abstract

The development of memristive devices is important for energy-efficient neuromorphic computing. While two-dimensional (2D) organic-inorganic hybrid perovskites offer structural tunability and improved stability, the correlation between their molecular-level interlayer architecture and resistive switching (RS) kinetics remains to be fully elucidated. Herein, we modulate the inorganic layer spacing in Dion-Jacobson (DJ) phase 2D perovskites, BDAPbI<sub>4</sub>, HDAPbI<sub>4</sub>, and ODAPbI<sub>4</sub>, by tailoring the alkyl chain length of diammonium ligands. The expanded interlayer environment regulates ion migration, resulting in improved RS behavior in HDAPbI<sub>4</sub> and ODAPbI<sub>4</sub> devices, with an ON/OFF ratio exceeding 10<sup>3</sup> and cycling endurance over 100 cycles. These devices emulate bioinspired synaptic functions, including the transition from short-term to long-term plasticity. Cross-Sim simulations of a three-layer neural network using the device conductance characteristics achieved a recognition accuracy of 96.6% for the MNIST data set, close to the software-defined benchmark of 98.2%. Overall, these results identify interlayer spacing as an important structural parameter that regulates ion migration, resistive switching behavior, and analog conductance modulation in 2D Dion-Jacobson perovskite memristors.