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Research output: Contribution to Journal/Magazine › Journal article › peer-review
Research output: Contribution to Journal/Magazine › Journal article › peer-review
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TY - JOUR
T1 - Quasi-Free Electron States Responsible for Single-Molecule Conductance Enhancement in Stable Radical
AU - Yang, Xingzhou
AU - Hou, Songjun
AU - Su, Meiling
AU - Zhan, Qian
AU - Zhang, Hanjun
AU - Quintero, Sergio M.
AU - Liu, Xiaodong
AU - Liu, Junyang
AU - Hong, Wenjing
AU - Casado, Juan
AU - Wu, Qingqing
AU - Lambert, Colin J.
AU - Zheng, Yonghao
PY - 2023/5/4
Y1 - 2023/5/4
N2 - 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.
AB - 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.
KW - General Materials Science
KW - Physical and Theoretical Chemistry
U2 - 10.1021/acs.jpclett.3c00536
DO - 10.1021/acs.jpclett.3c00536
M3 - Journal article
VL - 14
SP - 4004
EP - 4010
JO - The Journal of Physical Chemistry Letters
JF - The Journal of Physical Chemistry Letters
SN - 1948-7185
IS - 17
ER -