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Real-time observation of multiexcitonic states in ultrafast singlet fission using coherent 2D electronic spectroscopy
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Real-time observation of multiexcitonic states in ultrafast singlet fission using coherent 2D electronic spectroscopy
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Journal Article
Real-time observation of multiexcitonic states in ultrafast singlet fission using coherent 2D electronic spectroscopy
2016
Overview
Singlet fission is the spin-allowed conversion of a spin-singlet exciton into a pair of spin-triplet excitons residing on neighbouring molecules. To rationalize this phenomenon, a multiexcitonic spin-zero triplet-pair state has been hypothesized as an intermediate in singlet fission. However, the nature of the intermediate states and the underlying mechanism of ultrafast fission have not been elucidated experimentally. Here, we study a series of pentacene derivatives using ultrafast two-dimensional electronic spectroscopy and unravel the origin of the states involved in fission. Our data reveal the crucial role of vibrational degrees of freedom coupled to electronic excitations that facilitate the mixing of multiexcitonic states with singlet excitons. The resulting manifold of vibronic states drives sub-100 fs fission with unity efficiency. Our results provide a framework for understanding singlet fission and show how the formation of vibronic manifolds with a high density of states facilitates fast and efficient electronic processes in molecular systems.
Singlet fission, a spin-allowed conversion of a spin-singlet state into a pair of spin-triplet excitons, may be useful for the development of next-generation photovoltaics. Ultrafast coherence measurements now show that vibrational motions play a critical role in fission as they facilitate the mixing of triplet-pair states with singlet excitons.
Publisher
Nature Publishing Group UK,Nature Publishing Group
Subject
/ 140/125
/ 140/133
/ Atomic and Molecular Clusters
/ Condensed Matter Physics (including Material Physics, Nano Physics)
/ Den kondenserade materiens fysik (Här ingår: Materialfysik, nanofysik)
/ Fysik
/ Fysikalisk kemi (Här ingår: Yt- och kolloidkemi)
/ Kemi
/ Mesoscopic Systems and Quantum Hall Effect
/ Physical Chemistry (including Surface- and Colloid Chemistry)
/ Physics
