Theory of molecular conductance using a modular approach

Hsu, Liang-Yan; Rabitz, Herschel

doi:10.1063/1.4972131

Title: Theory of molecular conductance using a modular approach

Journal Article · Fri Dec 16 00:00:00 EST 2016 · Journal of Chemical Physics

DOI:https://doi.org/10.1063/1.4972131· OSTI ID:1465674

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Princeton Univ., NJ (United States). Dept. of Chemistry

This paper probes the correlation between the conductance of a molecular wire (the property of a whole system) and its constituent backbone units (modules). By using a tight-binding Hamiltonian combined with single-particle Green’s functions, we develop an approach that enables an estimate of a conductance decay constant in terms of the Hamiltonians of molecular backbone units and the couplings between two nearest-neighbor units in the off-resonant tunneling regime. For demonstration, we examine several representative molecular systems in a framework of the Hückel model (the simplest atomistic-level model). The Hückel model can be reduced to a single-orbital-per-site formulation [A. Nitzan, Annu. Rev. Phys. Chem. 52, 681 (2001)], and each energy level in the single-orbital-per-site picture can be expressed in an explicit form including the synergistic effect of all molecular orbitals of a molecular backbone unit. Finally, based on the proposed approach, we show the correspondence between the complete destructive quantum interference and an infinite injection gap and derive the preconditions of the modified Simmons equation and the rule of intramolecular series circuits.

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Research Organization:: Princeton Univ., NJ (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF); US Army Research Office (ARO)

Grant/Contract Number:: FG02-02ER15344; CHE-1058644; W911NF-13-1-0237

OSTI ID:: 1465674

Alternate ID(s):: OSTI ID: 1336499

Journal Information:: Journal of Chemical Physics, Vol. 145, Issue 23; ISSN 0021-9606

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 12 works

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