Quasi-Free Electron States Responsible for Single-Molecule Conductance Enhancement in Stable Radical

Autor: Xingzhou Yang, Songjun Hou, Meiling Su, Qian Zhan, Hanjun Zhang, Sergio M. Quintero, Xiaodong Liu, Junyang Liu, Wenjing Hong, Juan Casado, Qingqing Wu, Colin J. Lambert, Yonghao Zheng
Rok vydání: 2023
Předmět:
Zdroj: The Journal of Physical Chemistry Letters. 14:4004-4010
ISSN: 1948-7185
DOI: 10.1021/acs.jpclett.3c00536
Popis: Stable organic radicals, which possess half-filled orbitals in the vicinity of the Fermi energy, are promising candidates for electronic devices. In this Letter, using a combination of scanning-tunneling-microscopy-based break junction (STM-BJ) experiments and quantum transport theory, a stable fluorene-based radical is investigated. We demonstrate that the transport properties of a series of fluorene derivatives can be tuned by controlling the degree of localization of certain orbitals. More specifically, radical has a delocalized half-filled orbital resulting in Breit-Wigner resonances, leading to an unprecedented conductance enhancement of 2 orders of magnitude larger than the neutral nonradical counterpart ( ). In other words, conversion from a closed-shell fluorene derivative to the free radical in opens an electron transport path which massively enhances the conductance. This new understanding of the role of radicals in single-molecule junctions opens up a novel design strategy for single-molecule-based spintronic devices.
Databáze: OpenAIRE