Long-Lived Electronic Coherences from First Principles

Fuente: arXiv
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Autori principali: Suchan, Jiří, Levine, Benjamin G.
Natura: Preprint
Pubblicazione: 2025
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author Suchan, Jiří
Levine, Benjamin G.
author_facet Suchan, Jiří
Levine, Benjamin G.
contents Electronic coherences can be leveraged to control molecular dynamics, but such control is limited by ultrafast decoherence driven by coupling between electronic excitations and molecular vibrations. With the goal of understanding and controlling electronic coherence in molecules, we introduce a first-principles approach that enables direct simulation of the creation and decay of electronic coherences in molecules. Simulations of long-lived experimentally-observed coherences created upon multiphoton excitation of thiophene reveal coherent electronic motions within a dense manifold of Rydberg states, enabled by their relatively parallel potential energy surfaces.
format Preprint
id arxiv_https___arxiv_org_abs_2502_04494
institution arXiv
publishDate 2025
record_format arxiv
spellingShingle Long-Lived Electronic Coherences from First Principles
Suchan, Jiří
Levine, Benjamin G.
Chemical Physics
Electronic coherences can be leveraged to control molecular dynamics, but such control is limited by ultrafast decoherence driven by coupling between electronic excitations and molecular vibrations. With the goal of understanding and controlling electronic coherence in molecules, we introduce a first-principles approach that enables direct simulation of the creation and decay of electronic coherences in molecules. Simulations of long-lived experimentally-observed coherences created upon multiphoton excitation of thiophene reveal coherent electronic motions within a dense manifold of Rydberg states, enabled by their relatively parallel potential energy surfaces.
title Long-Lived Electronic Coherences from First Principles
topic Chemical Physics
url https://arxiv.org/abs/2502.04494