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Coherent singlet fission activated by symmetry breaking
- Source :
- Nature chemistry. 9(10)
- Publication Year :
- 2016
-
Abstract
- Singlet fission, in which a singlet exciton is converted to two triplet excitons, is a process that could be beneficial in photovoltaic applications. A full understanding of the dynamics of singlet fission in molecular systems requires detailed knowledge of the relevant potential energy surfaces and their (conical) intersections. However, obtaining such information is a nontrivial task, particularly for molecular aggregates. Here we investigate singlet fission in rubrene crystals using transient absorption spectroscopy and state-of-the-art quantum chemical calculations. We observe a coherent and ultrafast singlet-fission channel as well as the well-known and conventional thermally assisted incoherent channel. This coherent channel is accessible because the conical intersection for singlet fission on the excited-state potential energy surface is located very close to the equilibrium position of the ground-state potential energy surface and also because of the excitation of an intermolecular symmetry-breaking mode, which activates the electronic coupling necessary for singlet fission.
- Subjects :
- Chemistry
General Chemical Engineering
Exciton
02 engineering and technology
General Chemistry
Conical intersection
010402 general chemistry
021001 nanoscience & nanotechnology
01 natural sciences
Molecular physics
Potential energy
0104 chemical sciences
Excited state
Singlet fission
Potential energy surface
Symmetry breaking
0210 nano-technology
Excitation
Subjects
Details
- ISSN :
- 17554349
- Volume :
- 9
- Issue :
- 10
- Database :
- OpenAIRE
- Journal :
- Nature chemistry
- Accession number :
- edsair.doi.dedup.....9f990365bb12734da536f500a4b934f9