Work

Quantum electrodynamics formulation of multidimensional spectroscopy

Year: 2025

Type: article

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.

Source: The Journal of Chemical Physics

DOI: 10.1063/5.0267953

Author: Frank Schlawin

Institutions: Universität Hamburg, Max Planck Institute for the Structure and Dynamics of Matter, Hamburg Centre for Ultrafast Imaging

Language: English

Topic: Spectroscopy and Quantum Chemical Studies

Subfield: Atomic and Molecular Physics, and Optics

Field: Physics and Astronomy

Domain: Physical Sciences

Open Access status: hybrid

Estimated APC paid: $3,500

Funder: Deutsche Forschungsgemeinschaft