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

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.
Authors:
ORCiD logo [1] ; ORCiD logo [1]
  1. Univ. of California, San Diego, CA (United States). Dept. of Chemistry and Biochemistry
Publication Date:
Grant/Contract Number:
SC0006422
Type:
Accepted Manuscript
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 144; Journal Issue: 17; Journal ID: ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)
Research Org:
Univ. of California, San Diego, CA (United States)
Sponsoring Org:
USDOE Office of Science (SC)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
OSTI Identifier:
1471063
Alternate Identifier(s):
OSTI ID: 1251517