文献类型：期刊文献

英文题名：High-Performance Electrochemically Gated Single-Molecule Transistor Enabled by Interfacial Engineering

作者：Wang, Rui[1];Li, Yingjie[1];Yan, Siyu[1];Zhao, Yin[1];Tian, He[1];Li, Hongxiang[1]

机构：[1]East China Univ Sci & Technol, Feringa Nobel Prize Scientist Joint Res Ctr, Frontiers Sci Ctr Materiobiol & Dynam Chem, Inst Fine Chem,Sch Chem & Mol Engn,Key Lab Adv Mat, Shanghai 200237, Peoples R China

年份：2026

卷号：148

期号：4

起止页码：3987

外文期刊名：JOURNAL OF THE AMERICAN CHEMICAL SOCIETY

收录：;EI(收录号：20260820102049);WOS:【SCI-EXPANDED(收录号:WOS:001666645300001)】；

基金：This work was supported by the National Natural Science Foundation of China (grants 52273176, 22575084, 22405088, 22588101), Science and Technology Commission of Shanghai Municipality (grant No. 24DX1400200), the Fundamental Research Funds for the Central Universities, and East China University of Science and Technology.

语种：英文

外文关键词：Electrochemical electrodes - Energy gap - Field effect transistors - Molecules - Single electron transistors

摘要：Molecular-scale transistors, particularly those with high performance, are critical for advancing nanoelectronics toward practical applications. However, developing high-performance single-molecule transistor materials remains a significant challenge. Here, we design and synthesize a series of diketopyrrolopyrrole (DPP)-based narrow bandgap molecular wires with tailored molecule-electrode coupling. The molecular wire DPP-C-SMe, featuring electronic decoupling at the molecule-electrode interface, exhibits remarkable electrochemical gated modulation (>200-fold) and a low subthreshold swing (105 mV dec(-1)) within a 1 V potential window-significantly surpassing its coupled counterpart and ranking among the highest-performing single-molecule electrochemical transistors reported to date. Through combined conductance measurements, transition voltage spectroscopy (TVS), and DFT calculations, we elucidate that the electronic decoupling in DPP-C-SMe reduces the off-state conductance by lowering the low-bias transmission coefficient, while the preserved favorable energy alignment enables efficient nonresonant/near-resonant switching under electrochemical gating. This cooperative design principle is the key to its superior transistor performance. These findings provide a new strategic design principle that synergistically integrates a narrow-band gap molecular core with tailored interfacial engineering for high-performance single-molecule electrochemical transistors and advances the molecular-scale control of charge transport in functional nanoelectronics.