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QED_Isomerization.pdf (3.38 MB)

Investigate New Reactivities Enabled by Polariton Photochemistry

preprint
submitted on 04.06.2019, 00:05 and posted on 04.06.2019, 16:11 by Arkajit Mandal, Pengfei Huo
We perform quantum dynamics simulations to investigate new chemical reactivities enabled by cavity quantum electrodynamics. The quantum light-matter interactions between the molecule and the quantized radiation mode inside an optical cavity create a set of hybridized electronic-photonic states, so-called polaritons. The polaritonic states adapt the curvatures from both the ground and the excited electronic states, opening up new possibilities to control photochemical reactions by exploiting intrinsic quantum behaviors of light-matter interactions. With direct quantum dynamics simulations, we demonstrate that the selectivity of a model photo-isomerization reaction can be controlled by tuning the photon frequency of the cavity mode or the light-matter coupling strength, providing new ways to manipulate chemical reactions via light-matter interaction. We further investigate collective quantum effects enabled by coupling quantized radiation mode to multiple molecules. Our results suggest that in the resonance case, a photon is recycled among molecules to enable multiple excited state reactions, thus effectively functioning as a catalyst. In the non-resonance case, molecules emit and absorb virtual photons to initiate excited state reactions through fundamental quantum electrodynamics processes. These results from direct quantum dynamics simulations reveal basic principles of polariton photochemistry as well as promising reactivities that take advantage of intrinsic quantum behaviors of photons.

Funding

CHE-1836546

History

Email Address of Submitting Author

huo@chem.rochester.edu

Institution

University of Rochester

Country

United States

ORCID For Submitting Author

0000-0002-8639-9299

Declaration of Conflict of Interest

None

Exports