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Updated: May 27, 2025

High Resolution Phonon-assisted Quasi-resonance Fluorescence Spectroscopy
Published on: June 28, 2016
Nonlinear optical spectroscopy of open quantum systems
Haoran Sun1, Upendra Harbola2, Shaul Mukamel3
1Department of Chemistry and Biochemistry, University of California San Diego, La Jolla, California 92093, USA.
Abstract:
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.
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