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Title: Optical spectroscopy of molecular junctions: Nonequilibrium Green’s functions perspective

Abstract

We consider optical spectroscopy of molecular junctions from the quantum transport perspective when radiation field is quantized and optical response of the system is simulated as photon flux. Using exact expressions for photon and electronic fluxes derived within the nonequilibrium Green function (NEGF) methodology and utilizing fourth order diagrammatic perturbation theory (PT) in molecular coupling to radiation field, we perform simulations employing realistic parameters. Results of the simulations are compared to the bare PT which is usually employed in studies on nonlinear optical spectroscopy to classify optical processes. We show that the bare PT violates conservation laws, while flux conserving NEGF formulation mixes optical processes.

Authors:
;  [1]
  1. Department of Chemistry and Biochemistry, University of California San Diego, La Jolla, California 92093 (United States)
Publication Date:
OSTI Identifier:
22657958
Resource Type:
Journal Article
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 144; Journal Issue: 17; Other Information: (c) 2016 Author(s); Country of input: International Atomic Energy Agency (IAEA); Journal ID: ISSN 0021-9606
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; CONSERVATION LAWS; GREEN FUNCTION; NONLINEAR PROBLEMS; PERTURBATION THEORY; SIMULATION; SPECTROSCOPY

Citation Formats

Gao, Yi, and Galperin, Michael. Optical spectroscopy of molecular junctions: Nonequilibrium Green’s functions perspective. United States: N. p., 2016. Web. doi:10.1063/1.4948469.
Gao, Yi, & Galperin, Michael. Optical spectroscopy of molecular junctions: Nonequilibrium Green’s functions perspective. United States. https://doi.org/10.1063/1.4948469
Gao, Yi, and Galperin, Michael. 2016. "Optical spectroscopy of molecular junctions: Nonequilibrium Green’s functions perspective". United States. https://doi.org/10.1063/1.4948469.
@article{osti_22657958,
title = {Optical spectroscopy of molecular junctions: Nonequilibrium Green’s functions perspective},
author = {Gao, Yi and Galperin, Michael},
abstractNote = {We consider optical spectroscopy of molecular junctions from the quantum transport perspective when radiation field is quantized and optical response of the system is simulated as photon flux. Using exact expressions for photon and electronic fluxes derived within the nonequilibrium Green function (NEGF) methodology and utilizing fourth order diagrammatic perturbation theory (PT) in molecular coupling to radiation field, we perform simulations employing realistic parameters. Results of the simulations are compared to the bare PT which is usually employed in studies on nonlinear optical spectroscopy to classify optical processes. We show that the bare PT violates conservation laws, while flux conserving NEGF formulation mixes optical processes.},
doi = {10.1063/1.4948469},
url = {https://www.osti.gov/biblio/22657958}, journal = {Journal of Chemical Physics},
issn = {0021-9606},
number = 17,
volume = 144,
place = {United States},
year = {2016},
month = {5}
}

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Works referencing / citing this record:

Photonics and spectroscopy in nanojunctions: a theoretical insight
journal, January 2017


Simulation of optical response functions in molecular junctions
journal, June 2016


Nonequilibrium diagrammatic technique for Hubbard Green functions
journal, March 2017


On simulation of local fluxes in molecular junctions
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