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Title: Theory of molecular conductance using a modular approach

Abstract

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.

Authors:
ORCiD logo [1]; ORCiD logo [1]
  1. Princeton Univ., NJ (United States). Dept. of Chemistry
Publication Date:
Research Org.:
Princeton Univ., NJ (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); National Science Foundation (NSF); US Army Research Office (ARO)
OSTI Identifier:
1465674
Alternate Identifier(s):
OSTI ID: 1336499
Grant/Contract Number:  
FG02-02ER15344; CHE-1058644; W911NF-13-1-0237
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 145; Journal Issue: 23; Journal ID: ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
74 ATOMIC AND MOLECULAR PHYSICS; hopping transport; tunneling; eigenvalues; electrodes; transport properties; Green's function methods; Fermi levels; integrated circuits; quantum interference

Citation Formats

Hsu, Liang-Yan, and Rabitz, Herschel. Theory of molecular conductance using a modular approach. United States: N. p., 2016. Web. doi:10.1063/1.4972131.
Hsu, Liang-Yan, & Rabitz, Herschel. Theory of molecular conductance using a modular approach. United States. doi:10.1063/1.4972131.
Hsu, Liang-Yan, and Rabitz, Herschel. Fri . "Theory of molecular conductance using a modular approach". United States. doi:10.1063/1.4972131. https://www.osti.gov/servlets/purl/1465674.
@article{osti_1465674,
title = {Theory of molecular conductance using a modular approach},
author = {Hsu, Liang-Yan and Rabitz, Herschel},
abstractNote = {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.},
doi = {10.1063/1.4972131},
journal = {Journal of Chemical Physics},
number = 23,
volume = 145,
place = {United States},
year = {Fri Dec 16 00:00:00 EST 2016},
month = {Fri Dec 16 00:00:00 EST 2016}
}

Journal Article:
Free Publicly Available Full Text
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Cited by: 4 works
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Works referenced in this record:

Thermoelectricity in Molecular Junctions
journal, March 2007


Electronics using hybrid-molecular and mono-molecular devices
journal, November 2000

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