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Understanding the Role of Parallel Pathways via In-Situ Switching of Quantum Interference in Molecular Tunneling Junctions.


ABSTRACT: This study describes the modulation of tunneling probabilities in molecular junctions by switching one of two parallel intramolecular pathways. A linearly conjugated molecular wire provides a rigid framework that allows a second, cross-conjugated pathway to be effectively switched on and off by protonation, affecting the total conductance of the junction. This approach works because a traversing electron interacts with the entire quantum-mechanical circuit simultaneously; Kirchhoff's rules do not apply. We confirm this concept by comparing the conductances of a series of compounds with single or parallel pathways in large-area junctions using EGaIn contacts and single-molecule break junctions using gold contacts. We affect switching selectively in one of two parallel pathways by converting a cross-conjugated carbonyl carbon into a trivalent carbocation, which replaces destructive quantum interference with a symmetrical resonance, causing an increase in transmission in the bias window.

SUBMITTER: Soni S 

PROVIDER: S-EPMC7497014 | biostudies-literature | 2020 May

REPOSITORIES: biostudies-literature

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Understanding the Role of Parallel Pathways via In-Situ Switching of Quantum Interference in Molecular Tunneling Junctions.

Soni Saurabh S   Ye Gang G   Zheng Jueting J   Zhang Yanxi Y   Asyuda Andika A   Zharnikov Michael M   Hong Wenjing W   Chiechi Ryan C RC  

Angewandte Chemie (International ed. in English) 20200703 34


This study describes the modulation of tunneling probabilities in molecular junctions by switching one of two parallel intramolecular pathways. A linearly conjugated molecular wire provides a rigid framework that allows a second, cross-conjugated pathway to be effectively switched on and off by protonation, affecting the total conductance of the junction. This approach works because a traversing electron interacts with the entire quantum-mechanical circuit simultaneously; Kirchhoff's rules do no  ...[more]

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