TY - JOUR
T1 - High yield ultrafast intramolecular singlet exciton fission in a quinoidal bithiophene
AU - Varnavski, Oleg
AU - Abeyasinghe, Neranga
AU - Aragó, Juan
AU - Serrano-Pérez, Juan J.
AU - Ortí, Enrique
AU - López Navarrete, Juan T.
AU - Takimiya, Kazuo
AU - Casanova, David
AU - Casado, Juan
AU - Goodson, Theodore
N1 - Publisher Copyright:
© 2015 American Chemical Society.
PY - 2015/4/16
Y1 - 2015/4/16
N2 - We report the process of singlet exciton fission with high-yield upon photoexcitation of a quinoidal thiophene molecule. Efficient ultrafast triplet photogeneration and its yield are determined by photoinduced triplet-triplet absorption, flash photolysis triplet lifetime measurements, as well as by femtosecond time-resolved transient absorption and fluorescence methods. These experiments show that optically excited quinoidal bithiophene molecule undergoes ultrafast formation of the triplet-like state with the lifetime ∼57 μs. CASPT2 and RAS-SF calculations have been performed to support the experimental findings. To date, high singlet fission rates have been reported for crystalline and polycrystalline materials, whereas for covalently linked dimers and small oligomers it was found to be relatively small. In this contribution, we show an unprecedented quantum yield of intramolecular singlet exciton fission of ∼180% for a quinoidal bithiophene system.
AB - We report the process of singlet exciton fission with high-yield upon photoexcitation of a quinoidal thiophene molecule. Efficient ultrafast triplet photogeneration and its yield are determined by photoinduced triplet-triplet absorption, flash photolysis triplet lifetime measurements, as well as by femtosecond time-resolved transient absorption and fluorescence methods. These experiments show that optically excited quinoidal bithiophene molecule undergoes ultrafast formation of the triplet-like state with the lifetime ∼57 μs. CASPT2 and RAS-SF calculations have been performed to support the experimental findings. To date, high singlet fission rates have been reported for crystalline and polycrystalline materials, whereas for covalently linked dimers and small oligomers it was found to be relatively small. In this contribution, we show an unprecedented quantum yield of intramolecular singlet exciton fission of ∼180% for a quinoidal bithiophene system.
KW - Intramolecular
KW - Organic photovoltaics
KW - Quinoidal Oligothiophenes
KW - Singlet exciton fission
KW - Ultrafast spectroscopy
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U2 - 10.1021/acs.jpclett.5b00198
DO - 10.1021/acs.jpclett.5b00198
M3 - Article
AN - SCOPUS:84927920216
SN - 1948-7185
VL - 6
SP - 1375
EP - 1384
JO - Journal of Physical Chemistry Letters
JF - Journal of Physical Chemistry Letters
IS - 8
ER -