Non-adiabatic dynamics of molecules in optical cavities

Kowalewski, Markus; Bennett, Kochise; Mukamel, Shaul

doi:10.1063/1.4941053

Title: Non-adiabatic dynamics of molecules in optical cavities

Journal Article · Fri Feb 05 00:00:00 EST 2016 · Journal of Chemical Physics

DOI:https://doi.org/10.1063/1.4941053· OSTI ID:1469202

^[1]; Bennett, Kochise ^[1]; Mukamel, Shaul ^[1]

Univ. of California, Irvine, CA (United States)

Strong coupling of molecules to the vacuum field of micro cavities can modify the potential energy surfaces thereby opening new photophysical and photochemical reaction pathways. While the influence of laser fields is usually described in terms of classical field, coupling to the vacuum state of a cavity has to be described in terms of dressed photon-matter states (polaritons) which require quantized fields. We present a derivation of the non-adiabatic couplings for single molecules in the strong coupling regime suitable for the calculation of the dressed state dynamics. The formalism allows to use quantities readily accessible from quantum chemistry codes like the adiabatic potential energy surfaces and dipole moments to carry out wave packet simulations in the dressed basis. In conclusion, the implications for photochemistry are demonstrated for a set of model systems representing typical situations found in molecules.

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Research Organization:: Univ. of California, Irvine, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division

Grant/Contract Number:: FG02-04ER15571

OSTI ID:: 1469202

Alternate ID(s):: OSTI ID: 1236993

Journal Information:: Journal of Chemical Physics, Vol. 144, Issue 5; ISSN 0021-9606

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 110 works

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