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Two-Dimensional Spectroscopy of Open Quantum Systems: Nonequilibrium Green's Function Formulation
Haoran Sun1, Upendra Harbola2, Shaul Mukamel3
1Department of Chemistry & Biochemistry, University of California San Diego, La Jolla, California 92093, United States.
The Journal of Physical Chemistry Letters
|February 18, 2025
Summary
This study develops two-dimensional spectroscopy for open quantum systems, combining photon flux and electron current measurements. The new theory, validated by simulations, enables simultaneous analysis of optical and transport phenomena in junctions.
Area of Science:
- Quantum physics
- Spectroscopy
- Condensed matter physics
Background:
- Open quantum systems present challenges for characterization due to environmental interactions.
- Simultaneous measurement of multiple fluxes (e.g., optical and electronic) is crucial for understanding complex quantum phenomena.
- Existing spectroscopic techniques often lack the capability to probe multiple correlated dynamics concurrently.
Purpose of the Study:
- To develop a theoretical framework for two-dimensional spectroscopy applicable to open quantum systems with multiple measurable fluxes.
- To integrate optical measurements (photon flux) with transport measurements (electron currents) within a unified spectroscopic approach.
- To provide a method for simultaneously analyzing correlated quantum dynamics across different measurement domains.
Main Methods:
- Development of a nonself-consistent nonequilibrium Green's function formulation.
- Extension of two-dimensional spectroscopy theory to accommodate concurrent photon flux and electron current measurements.
- Numerical simulations utilizing a generic junction model to demonstrate theoretical derivations.
Main Results:
- A comprehensive theory for two-dimensional spectroscopy of open quantum systems with multiple fluxes has been established.
- The framework successfully integrates optical and electronic measurements, enabling simultaneous probing of photon and electron dynamics.
- Numerical simulations confirm the validity and applicability of the developed theoretical approach.
Conclusions:
- The presented two-dimensional spectroscopy method offers a powerful new tool for investigating complex quantum phenomena in open systems.
- This approach facilitates a deeper understanding of the interplay between optical and charge transport properties in nanoscale junctions.
- The theoretical framework and simulation results pave the way for experimental advancements in correlated quantum measurements.
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