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Manipulating nonadiabatic conical intersection dynamics by optical cavities

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Abstract

Optical cavities hold great promise to manipulate and control the photochemistry of molecules. We demonstrate how molecular photochemical processes can be manipulated by strong light–matter coupling. For a molecule with an inherent conical intersection, optical cavities can induce significant changes in the nonadiabatic dynamics by either splitting the pristine conical intersections into two novel polaritonic conical intersections or by creating light-induced avoided crossings in the polaritonic surfaces. This is demonstrated by exact real-time quantum dynamics simulations of a three-state two-mode model of pyrazine strongly coupled to a single cavity photon mode. We further explore the effects of external environments through dissipative polaritonic dynamics computed using the hierarchical equation of motion method. We find that cavity-controlled photochemistry can be immune to external environments. We also demonstrate that the polariton-induced changes in the dynamics can be monitored by transient absorption spectroscopy.

Graphical abstract: Manipulating nonadiabatic conical intersection dynamics by optical cavities

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Supplementary files

Article information


Submitted
04 Oct 2019
Accepted
12 Dec 2019
First published
12 Dec 2019

This article is Open Access
All publication charges for this article have been paid for by the Royal Society of Chemistry

Chem. Sci., 2020, Advance Article
Article type
Edge Article

Manipulating nonadiabatic conical intersection dynamics by optical cavities

B. Gu and S. Mukamel, Chem. Sci., 2020, Advance Article , DOI: 10.1039/C9SC04992D

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