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

Gao, Yi; Galperin, Michael

doi:10.1063/1.4948469

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

Journal Article · Fri May 06 00:00:00 EDT 2016 · Journal of Chemical Physics

DOI:https://doi.org/10.1063/1.4948469· OSTI ID:1471063

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Univ. of California, San Diego, CA (United States). Dept. of Chemistry and Biochemistry

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. Lastly, we show that the bare PT violates conservation laws, while flux conserving NEGF formulation mixes optical processes.

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Research Organization:: Univ. of California, San Diego, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC)

Grant/Contract Number:: SC0006422

OSTI ID:: 1471063

Alternate ID(s):: OSTI ID: 1251517

Journal Information:: Journal of Chemical Physics, Vol. 144, Issue 17; ISSN 0021-9606

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

Country of Publication:: United States

Language:: English

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Cited by: 17 works

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