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Nonlinear optical spectroscopy of open quantum systems.

Haoran Sun1, Upendra Harbola2, Shaul Mukamel3

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Single-molecule spectroscopy and molecular electronics intersect, revealing connections between optical spectroscopy and nonequilibrium Green's functions. Analyzing open quantum systems requires the Green's function framework for accurate molecular electronics research.

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Area of Science:

  • Physical Chemistry
  • Molecular Electronics
  • Spectroscopy

Background:

  • Nanoscale experimental techniques enable single-molecule spectroscopy on current-carrying junctions.
  • This research bridges optical spectroscopy and molecular electronics.
  • Existing methods for molecular electronics often use nonequilibrium Green's functions (NEGF).

Purpose of the Study:

  • To pedagogically compare standard nonlinear optical spectroscopy with the NEGF method.
  • To highlight similarities and differences between these theoretical frameworks.
  • To establish the necessity of the Green's function framework for optical spectroscopy of open quantum systems.

Main Methods:

  • Perturbation theory expansion of standard nonlinear optical spectroscopy.
  • Perturbative diagrammatic formulation of NEGF.
  • Comparative analysis of the two theoretical approaches.

Main Results:

  • Identified similarities and differences between optical spectroscopy and NEGF perturbation theories.
  • Demonstrated the applicability of Green's function formalism to optical spectroscopy.
  • Provided a unified theoretical perspective.

Conclusions:

  • The Green's function framework offers a more general and robust approach for analyzing optical spectroscopy in open quantum systems.
  • This comparison enhances understanding at the intersection of optical spectroscopy and molecular electronics.
  • Future research in molecular electronics can benefit from this integrated theoretical perspective.