Rights statement: This is the author’s version of a work that was accepted for publication in Matter. Changes resulting from the publishing process, such as peer review, editing, corrections, structural formatting, and other quality control mechanisms may not be reflected in this document. Changes may have been made to this work since it was submitted for publication. A definitive version was subsequently published in Matter, 4, 11, 2021 DOI: 10.1016/j.matt.2021.08.016
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Final published version
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 - Promotion and suppression of single-molecule conductance by quantum interference in macrocyclic circuits
AU - Chen, Hongliang
AU - Hou, Songjun
AU - Wu, Qingqing
AU - Jiang, Feng
AU - Zhou, Ping
AU - Zhang, Long
AU - Jiao, Yang
AU - Song, Bo
AU - Guo, Qing-Hui
AU - Chen, Xiao-Yang
AU - Hong, Wenjing
AU - Lambert, Colin
AU - Stoddart, J. Fraser
N1 - This is the author’s version of a work that was accepted for publication in Matter. Changes resulting from the publishing process, such as peer review, editing, corrections, structural formatting, and other quality control mechanisms may not be reflected in this document. Changes may have been made to this work since it was submitted for publication. A definitive version was subsequently published in Matter, 4, 11, 2021 DOI: 10.1016/j.matt.2021.08.016
PY - 2021/11/30
Y1 - 2021/11/30
N2 - Single-molecule electronics is a sub-field of nanoelectronics in which individual devices are formed from single molecules placed between source and drain electrodes. During the past few years, scientists have demonstrated that the flow of electricity through these devices is controlled by quantum interference (QI) between electrons passing from source to drain. Their future development, however, is hampered by difficulties in controlling interference effects. Herein, we demonstrate that electron transport in tetracationic cyclophane circuits is mediated by QI between channels formed from two lowest unoccupied molecular orbitals (LUMOs), while their highest occupied molecular orbitals (HOMOs) play no significant role. Energy differences between these two LUMO channels induce constructive interference, leading to high conductance. By contrast, phase differences between these LUMO channels result in destructive interference and a suppression in overall conductance. Such a design of single-molecule circuits enables the construction of single-molecule conductors and insulators based on a single cyclophane platform.
AB - Single-molecule electronics is a sub-field of nanoelectronics in which individual devices are formed from single molecules placed between source and drain electrodes. During the past few years, scientists have demonstrated that the flow of electricity through these devices is controlled by quantum interference (QI) between electrons passing from source to drain. Their future development, however, is hampered by difficulties in controlling interference effects. Herein, we demonstrate that electron transport in tetracationic cyclophane circuits is mediated by QI between channels formed from two lowest unoccupied molecular orbitals (LUMOs), while their highest occupied molecular orbitals (HOMOs) play no significant role. Energy differences between these two LUMO channels induce constructive interference, leading to high conductance. By contrast, phase differences between these LUMO channels result in destructive interference and a suppression in overall conductance. Such a design of single-molecule circuits enables the construction of single-molecule conductors and insulators based on a single cyclophane platform.
KW - Cyclophanes
KW - Intramolecular circuits
KW - LUMO-dominated transport
KW - Molecular electronics
KW - Quantum interference
KW - Single-supermolecule electronics
KW - STM-BJs
U2 - 10.1016/j.matt.2021.08.016
DO - 10.1016/j.matt.2021.08.016
M3 - Journal article
VL - 4
SP - 3662
EP - 3676
JO - Matter
JF - Matter
IS - 11
ER -