Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 141, Issue 44, Pages 17558-17570Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jacs.9b05561
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Funding
- Engineering and Physical Sciences Research Council, U.K. [EP/L015552/1, EP/M025330/1, EP/M005143/1]
- Winton Programme for the Physics of Sustainability
- A*STAR Singapore
- Jesus College, Cambridge, U.K.
- National Science Foundation [CHE-1555205]
- MOE Tier 3 programme [MOE2014-T3-1-004]
- EPSRC [EP/M005143/1, EP/M025330/1] Funding Source: UKRI
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Singlet fission in organic semiconductors causes a singlet exciton to decay into a pair of triplet excitons and holds potential for increasing the efficiency of photovoltaic devices. In this combined experimental and theoretical study, we reveal that a covalent dimer of the organic semiconductor tetracene undergoes activated singlet fission by qualitatively different mechanisms depending on the solvent environment. We show that intramolecular vibrations are an integral part of this mechanism, giving rise to mixing between charge transfer and triplet pair excitations. Either coherent or incoherent singlet fission can occur, depending on the transient solvent-induced energetic proximity between the states, giving rise to complex variation of the singlet fission mechanism and time scale in the different environments. Our results suggest a more general principle for controlling the efficiency of photochemical reactions by utilizing transient interactions to tune the energetics of reactant and product states and switch between incoherent and coherent dynamics.
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