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Updated: May 9, 2025

High Resolution Phonon-assisted Quasi-resonance Fluorescence Spectroscopy
Published on: June 28, 2016
Quantum electrodynamics formulation of multidimensional spectroscopy
1Max Planck Institute for the Structure and Dynamics of Matter, Luruper Chaussee 149, 22761 Hamburg, Germany; University of Hamburg, Luruper Chaussee 149, Hamburg, Germany; and The Hamburg Centre for Ultrafast Imaging, Luruper Chaussee 149, Hamburg D-22761, Germany.
Abstract:
We present a description of multidimensional spectroscopy, where all the light pulses are treated quantum-mechanically and the signal is expressed as a quantum dynamical map of the broadband light fields. Focusing in particular on the rephasing contribution to two-dimensional spectroscopy, we demonstrate how the semiclassical description emerges naturally as a limiting case of the quantum description. Our work establishes a formalism to apply quantum information methods to the optimization of multidimensional spectroscopy and address, e.g., fundamental resolution limits from a quantum metrological perspective.
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