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Singlet Fission Of Amorphous Rubrene Modulated By Polariton Formation

JOURNAL OF CHEMICAL PHYSICS(2019)

引用 34|浏览10
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摘要
The excited-state dynamics of molecular aggregates are governed by their potential energy landscape that can hardly be controlled artificially. However, it is possible to alter the excited state dynamics by a strong coupling between light and molecules (polariton formation) because it can decouple the electronic and vibrational degrees of freedom. Here, we demonstrate this polaron decoupling effect on the photochemical dynamics in singlet fission (SF) of amorphous rubrene thin films embedded in optical microcavities. The vibronic feature of polariton states in this system is characterized through the analysis of steady state absorption spectra by using the Holstein-Tavis-Cummings model. On the basis of this analysis, we show with time-resolved spectroscopy that the SF rate following a resonant excitation of the lowest energy polariton state is indeed modulated when the cavity photon energy is changed. A numerical simulation by using Fermi's golden rule formula with the vibronic polariton feature successfully accounts for the observed modulation of the SF rate, indicating that the polaron decoupling plays a decisive role in the nonadiabatic dynamics.
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关键词
amorphous rubrene,polariton formation,singlet fission
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