Insights into the Mechanism of Intramolecular Singlet Fission: An Electronic Structure Study using Multireference Perturbation Theory Methods
Pedro B. Coto a, Seelam Rajagopala Reddy a, Michael Thoss a
a Friedrich Alexander Universtät Erlangen-Nürnberg, Staudtstrasse 7 / B2, Erlangen, 91058, Germany
Asia-Pacific International Conference on Perovskite, Organic Photovoltaics and Optoelectronics
Proceedings of International Conference Asia-Pacific Hybrid and Organic Photovoltaics (AP-HOPV17)
Yokohama-shi, Japan, 2017 February 2nd - 4th
Organizers: Tsutomu Miyasaka and Iván Mora-Seró
Oral, Pedro B. Coto, presentation 072
Publication date: 7th November 2016

Singlet fission (SF) is a mechanism where two triplet excitons are formed after photoexcitation of a singlet exciton through a spin-allowed process.1 This process has received great attention recently as it has the potential to circumvent the Shockley-Queisser efficiency limit exhibited by single layer solar cells.2 In this contribution, we report the results obtained in the investigation of the mechanism of intramolecular SF in pentacene oligomers employing multireference perturbation theory and quantum dynamics methods.3,4 Specifically, we have investigated a series of 6,13-bis(triisopropylsilylethynyl)pentacene dimers covalently bonded to a phenylene spacer in ortho, meta, and para conformations. The results point out the fundamental role of charge transfer states in the mechanism of SF. In particular, it is shown that mixing between the absorbing excited state and higher-lying charge transfer states via a superexchange-like mechanism facilitates SF. The role that the electronic structure of the linker has in the control of intramolecular SF is also discussed.



1. M. B. Smith, J. Michl, Chem. Rev. 2010, 110, 6891.

2. W. Shockley, H. J. Queisser, J. Appl. Phys. 1961, 32, 510.

3. J. Zirzlmeier, D. Lehnherr, P. B. Coto, E. T. Chernick, R. Casillas, B. Basel, M. Thoss, R. R. Tykwinski, D. M. Guldi, Proc. Natl. Acad. Sci. (USA) 2015, 112, 5325.

4. J. Zirzlmeier, R. Casillas, S. R. Reddy, P. B. Coto, D. Lehnherr, E. T. Chernick, I. Papadopoulos, M. Thoss, R. R. Tykwinski, D. M. Guldi, Nanoscale, 2016, 8, 10113.

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