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<p>The precise engineering of nanoscale gaps between discrete building blocks offers a direct pathway to govern charge transport physics in functional materials. Here, we demonstrate a fundamental transition from stochastic bulk conduction to reliable interface-mediated volatile switching by deliberately introducing structural discontinuity in spinel-type Co<sub>3</sub>O<sub>4</sub> nanocube (NC) arrays. While continuous oxide thin films suffer from irreversible breakdown and featureless transport, and disordered NC assemblies exhibit only leakage-like conduction, our self-assembled NC architecture enables a stable and low-power functional response. Utilizing an automated metrology framework based on the Segment Anything Model (SAM), we confirm the formation of a highly ordered, non-percolated square lattice with a narrowly distributed interparticle gap of 2.84 ± 0.64&#xa0;nm across thousands of junctions. This statistically defined NC-gap-NC junction network confines the active conduction volume to nanoscale junctions, achieving an ultralow operating current of ~ 10 nA and exceptional statistical uniformity (coefficient of variation &lt; 9%); the operating voltage is likewise set by the interparticle junction and can be brought to the ~ 1&#xa0;V regime by contracting the gap through ligand exchange. Quantitative analysis identifies junction-limited, multi-regime transport across the NC-gap-NC interfaces as the dominant conduction picture, with Schottky-emission-like injection at intermediate fields and Fowler–Nordheim-type field-assisted tunneling at high fields. Furthermore, time-resolved measurements reveal dual-mode relaxation dynamics characterized by microsecond electronic detrapping and slow recovery consistent with ionic back-diffusion, which facilitate complex temporal dynamics for biomimetic signal processing. Our findings suggest that a preformed, statistically quantified nanogap network, rather than bulk percolation, can serve as a useful design principle for energy-efficient electronic primitives beyond conventional continuous media.</p>

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Engineering structural discontinuity in ordered Co3O4 nanocube arrays for volatile memristive dynamics

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年7月30日

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  • Inhyeok Oh,
  • Jun Beom Hwang,
  • Minwoo Kang,
  • Daehyeok Kim,
  • Seohyeon Kim,
  • Jungdae Lee,
  • Hyeon Kim,
  • Donghyeon Lee,
  • Myoung Hwan Oh,
  • Sanghan Lee

摘要

The precise engineering of nanoscale gaps between discrete building blocks offers a direct pathway to govern charge transport physics in functional materials. Here, we demonstrate a fundamental transition from stochastic bulk conduction to reliable interface-mediated volatile switching by deliberately introducing structural discontinuity in spinel-type Co3O4 nanocube (NC) arrays. While continuous oxide thin films suffer from irreversible breakdown and featureless transport, and disordered NC assemblies exhibit only leakage-like conduction, our self-assembled NC architecture enables a stable and low-power functional response. Utilizing an automated metrology framework based on the Segment Anything Model (SAM), we confirm the formation of a highly ordered, non-percolated square lattice with a narrowly distributed interparticle gap of 2.84 ± 0.64 nm across thousands of junctions. This statistically defined NC-gap-NC junction network confines the active conduction volume to nanoscale junctions, achieving an ultralow operating current of ~ 10 nA and exceptional statistical uniformity (coefficient of variation < 9%); the operating voltage is likewise set by the interparticle junction and can be brought to the ~ 1 V regime by contracting the gap through ligand exchange. Quantitative analysis identifies junction-limited, multi-regime transport across the NC-gap-NC interfaces as the dominant conduction picture, with Schottky-emission-like injection at intermediate fields and Fowler–Nordheim-type field-assisted tunneling at high fields. Furthermore, time-resolved measurements reveal dual-mode relaxation dynamics characterized by microsecond electronic detrapping and slow recovery consistent with ionic back-diffusion, which facilitate complex temporal dynamics for biomimetic signal processing. Our findings suggest that a preformed, statistically quantified nanogap network, rather than bulk percolation, can serve as a useful design principle for energy-efficient electronic primitives beyond conventional continuous media.