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Quantum Control of Ultrafast Internal Conversion using Nano-Confined Virtual Photons

submitted on 26.11.2019, 05:47 and posted on 29.11.2019, 19:13 by Aleksandr Avramenko, Aaron Rury

The rational control of non-radiative relaxation remains an unfulfilled goal for synthetic chemistry. In this study, we show strongly coupling an ensemble of molecules to the virtual photons of an electromagnetic cavity provides a rational handle over ultrafast, non-radiative dynamics. Specifically, we control the concentration of zinc tetraphenyl porphyrin molecules within nano-scale Fabry-Perot cavity structures to show a variable collective vacuum Rabi splitting between the polaritons coincides with changes in internal conversion rates. We find these changes obey a power law dependence on the collective vacuum Rabi splitting, but de- viate from the predictions of so-called gap laws. We also show simple theories of structural changes caused by polariton formation cannot explain discrepancies between our results and established theoretical predictions. Our results demonstrate a mechanism by which cavity polariton formation controls the fundamental photo-physics of light harvesting and photo- catalytic molecular moieties and the gap remaining in our fundamental understanding of these mechanisms.


Email Address of Submitting Author


Wayne State University


United States of America

ORCID For Submitting Author


Declaration of Conflict of Interest

No conflict