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Title: Nonlinear optical spectroscopy of open quantum systems
The development of experimental techniques at the nanoscale has enabled the performance of spectroscopic measurements on single-molecule current-carrying junctions. These experiments serve as a natural intersection for the research fields of optical spectroscopy and molecular electronics. We present a pedagogical comparison between the perturbation theory expansion of standard nonlinear optical spectroscopy and the (non-self-consistent) perturbative diagrammatic formulation of the nonequilibrium Green’s functions method (which is widely used in molecular electronics), highlighting their similarities and differences. By comparing the two approaches, we argue that the optical spectroscopy of open quantum systems must be analyzed within the more general Green’s function framework.  more » « less
Award ID(s):
2246379 2154323
PAR ID:
10572575
Author(s) / Creator(s):
; ; ;
Publisher / Repository:
American Institute of Physics
Date Published:
Journal Name:
The Journal of Chemical Physics
Volume:
162
Issue:
7
ISSN:
0021-9606
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
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