文献类型：期刊文献

英文题名：Integration of Photoresponsive Single-Molecule Bithermoelectric Devices

作者：Fang, Chao[1,2];Wang, Siwen[1,2];Liang, Mingchen[1,2];Gan, Jinyu[1,2];Ji, Shurui[1,2];Yan, Chenshuai[1,2];Cao, Ning[1,2];Shi, Jia[1,2];Zou, Qi[3,4];Liu, Junyang[1,2];Hong, Wenjing[1,2]

机构：[1]Xiamen Univ, Coll Chem & Chem Engn, State Key Lab Phys Chem Solid Surfaces, Xiamen 361005, Peoples R China;[2]Xiamen Univ, Inst Artificial Intelligence, Innovat Lab Sci & Technol Energy Mat Fujian Prov I, Xiamen 361005, Peoples R China;[3]East China Univ Sci & Technol, Key Lab Adv Mat, Shanghai 200237, Peoples R China;[4]East China Univ Sci & Technol, Feringa Nobel Prize Scientist Joint Res Ctr, Frontiers Sci Ctr Materiobiol & Dynam Chem, Sch Chem & Mol Engn, Shanghai 200237, Peoples R China

年份：2026

卷号：148

期号：3

起止页码：3383

外文期刊名：JOURNAL OF THE AMERICAN CHEMICAL SOCIETY

收录：;EI(收录号：20260720046086);WOS:【SCI-EXPANDED(收录号:WOS:001661038700001)】；

基金：We are grateful for financial support from the National Key R and D Program of China (2024YFA1208103), the National Natural Science Foundation of China (Nos. 92577106, 22173075, 22325303, 22250003, 22475068), the Fujian Provincial Department of Science and Technology (2023H6002), and the Science and Technology Commission of Shanghai Municipality (No. 24DX1400200)

语种：英文

外文关键词：Density functional theory - Electron energy levels - Molecules - Thermoelectric energy conversion - Thermoelectric equipment - Thermoelectric power

摘要：Organic thermoelectric materials capable of converting heat into electricity become important for sustainable energy conversion. Single-molecule thermoelectric devices present a promising opportunity for high-efficiency thermopower conversion by precisely controlling molecular energy levels, which induces energy-dependent transport asymmetry and consequently enhances the Seebeck coefficient. However, scalable thermopower output remains constrained by the challenges of assembling heteromolecular thermoelectric units with opposite polarities, whereas dynamic in situ control over the polarity of the Seebeck coefficient offers a feasible strategy for overcoming this limitation. Here, we report a photoresponsive single-molecule bithermoelectric device based on dithienylethene (DTE) derivatives using the scanning tunneling microscope break-junction (STM-BJ) technique with a thermoelectric module. The Seebeck coefficient could be reversibly switched between positive (P-type) and negative (N-type) values upon respective UV and visible light irradiation, as confirmed by thermoelectric measurements and density functional theory (DFT) calculations. By assembling an array of DTE monolayer with an optical mask to partially trigger the photoisomerization, we experimentally realized alternating P-type and N-type DTE molecular junctions connected through interleaved top and bottom electrodes, yielding a series-integrated molecular thermoelectric device with an amplified thermopower output over 9000 mu V under a temperature gradient of 30 K. This study presents a viable strategy for realizing programmable and scalable molecular thermoelectrics by utilizing photoswitchable bithermoelectric molecular devices.