Strong coupling electron-photon dynamics: A real-time investigation of energy redistribution in molecular polaritons

Author:

Castagnola Matteo1ORCID,Lexander Marcus T.1ORCID,Ronca Enrico2ORCID,Koch Henrik1ORCID

Affiliation:

1. Norwegian University of Science and Technology

2. Università degli Studi di Perugia

Abstract

We analyze the real-time electron-photon dynamics in long- and short-range energy transfer using a real-time quantum electrodynamics coupled cluster model, which allows for spatial and temporal visualization of transport processes. We compute the time evolution of photonic and molecular observables, such as the dipole moment and the photon coordinate, following the excitation of the system induced by short laser pulses. Our simulations show that intermolecular interactions and light-matter strong coupling lead to modified electronic polarization compared to the undressed molecules. The developed method can simulate multiple high-intensity laser pulses while explicitly retaining electronic and electron-photon correlation and is thus suited for nonlinear optics and transient absorption spectroscopies of molecular polaritons. Published by the American Physical Society 2024

Funder

European Research Council

Horizon 2020

Norges Teknisk-Naturvitenskapelige Universitet

Publisher

American Physical Society (APS)

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