Indirect Probing of Light-Induced Nonadiabatic Dynamics in Lossy Nanocavities

Light-induced nonadiabatic effects can arise from the interaction of a molecule with the quantized electromagnetic field of a Fabry–Pérot or plasmonic nanocavity. In this context, the quantized radiation field mixes the vibrational, rotational, and electronic degrees of freedom. In this work, we investigate the photodissociation dynamics of a rotating hydrogen molecule within a lossy plasmonic nanocavity. We highlight that, due to significant cavity loss, the dynamics are governed by an infinite number of light-induced conical intersections. We also examine the dissociation dynamics of fixed-in-space molecules by neglecting rotation, employing both the Lindblad master and non-Hermitian lossy Schrödinger equations. Additionally, we incorporate the effects of rotation within the parameter range of perfect agreement using the non-Hermitian lossy Schrödinger method. Furthermore, we show that in the absence of photon losses, there is a close correspondence between the classical Floquet description and the radiation field model.

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Publication Details

Journal
The Journal of Physical Chemistry C
Published
2025-03-13
DOI
https://doi.org/10.1021/acs.jpcc.5c01367
Primary Topic
Strong Light-Matter Interactions
Type
article
Field-Weighted Citation Impact
0.00

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article

Indirect Probing of Light-Induced Nonadiabatic Dynamics in Lossy Nanocavities

Csaba Fábri, Ágnes Vibók, Gábor J. Halász, Krisztián Szabó
The Journal of Physical Chemistry C
Strong Light-Matter Interactions
article

Indirect Probing of Light-Induced Nonadiabatic Dynamics in Lossy Nanocavities

Csaba Fábri, Ágnes Vibók, Gábor J. Halász, Krisztián Szabó
article en

Abstract

Light-induced nonadiabatic effects can arise from the interaction of a molecule with the quantized electromagnetic field of a Fabry–Pérot or plasmonic nanocavity. In this context, the quantized radiation field mixes the vibrational, rotational, and electronic degrees of freedom. In this work, we investigate the photodissociation dynamics of a rotating hydrogen molecule within a lossy plasmonic nanocavity. We highlight that, due to significant cavity loss, the dynamics are governed by an infinite number of light-induced conical intersections. We also examine the dissociation dynamics of fixed-in-space molecules by neglecting rotation, employing both the Lindblad master and non-Hermitian lossy Schrödinger equations. Additionally, we incorporate the effects of rotation within the parameter range of perfect agreement using the non-Hermitian lossy Schrödinger method. Furthermore, we show that in the absence of photon losses, there is a close correspondence between the classical Floquet description and the radiation field model.

The Journal of Physical Chemistry CVol. 129(12)
University of Debrecen (HU), ELI-HU Research and Development Non-Profit (HU)
Magyar Tudományos Akadémia, Debreceni Egyetem, Nemzeti Kutatási, Fejlesztési és Innovaciós Alap
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Strong Light-Matter Interactions
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Indirect Probing of Light-Induced Nonadiabatic Dynamics in Lossy Nanocavities — Csaba Fábri, Ágnes Vibók, et al. · The Journal of Physical Chemistry C (2025) | TGRS Research Map | TGRS