Li Jinshi, Shen Pingchuan, Zhuang Zeyan, Wu Junqi, Tang Ben Zhong, Zhao Zujin
State Key Laboratory of Luminescent Materials and Devices, Guangdong Provincial Key Laboratory of Luminescence from Molecular Aggregates, South China University of Technology, Guangzhou, 510640, China.
School of Science and Engineering, Shenzhen Institute of Aggregate Science and Technology, The Chinese University of Hong Kong, Shenzhen, Guangdong, 518172, China.
Nat Commun. 2023 Oct 6;14(1):6250. doi: 10.1038/s41467-023-42028-5.
Voltage-gated processing units are fundamental components for non-von Neumann architectures like memristor and electric synapses, on which nanoscale molecular electronics have possessed great potentials. Here, tailored foldamers with furan‒benzene stacking (f-Fu) and thiophene‒benzene stacking (f-Th) are designed to decipher electro-responsive through-space interaction, which achieve volatile memory behaviors via quantum interference switching in single-molecule junctions. f-Fu exhibits volatile turn-on feature while f-Th performs stochastic turn-off feature with low voltages as 0.2 V. The weakened orbital through-space mixing induced by electro-polarization dominates stacking malposition and quantum interference switching. f-Fu possesses higher switching probability and faster responsive time, while f-Th suffers incomplete switching and longer responsive time. High switching ratios of up to 91 for f-Fu is realized by electrochemical gating. These findings provide evidence and interpretation of the electro-responsiveness of non-covalent interaction at single-molecule level and offer design strategies of molecular non-von Neumann architectures like true random number generator.
电压门控处理单元是忆阻器和电突触等非冯·诺依曼架构的基本组件，纳米级分子电子学在这些架构上具有巨大潜力。在此，设计了具有呋喃-苯堆积（f-Fu）和噻吩-苯堆积（f-Th）的定制折叠体，以解读电响应性的空间相互作用，其通过单分子结中的量子干涉开关实现易失性存储行为。f-Fu表现出易失性开启特性，而f-Th在0.2 V的低电压下表现出随机关闭特性。由电极化引起的轨道空间混合减弱主导了堆积错位和量子干涉开关。f-Fu具有更高的开关概率和更快的响应时间，而f-Th则存在不完全开关和更长的响应时间。通过电化学门控实现了f-Fu高达91的高开关比。这些发现为单分子水平上非共价相互作用的电响应性提供了证据和解释，并为诸如真随机数发生器等分子非冯·诺依曼架构提供了设计策略。
