Effect of high-frequency modes on singlet fission dynamics
Date of Issue2017
School of Materials Science and Engineering
Singlet fission is a spin-allowed energy conversion process whereby a singlet excitation splits into two spin-correlated triplet excitations residing on adjacent molecules and has a potential to dramatically increase the efficiency of organic photovoltaics. Recent time-resolved nonlinear spectra of pentacene derivatives have shown the importance of high frequency vibrational modes in efficient fission. In this work, we explore impacts of vibration-induced fluctuations on fission dynamics through quantum dynamics calculations with parameters from fitting measured linear and nonlinear spectra. We demonstrate that fission dynamics strongly depends on the frequency of the intramolecular vibrational mode. Furthermore, we examine the effect of two vibrational modes on fission dynamics. Inclusion of a second vibrational mode creates an additional fission channel even when its Huang-Rhys factor is relatively small. Addition of more vibrational modes may not enhance the fission per se, but can dramatically affect the interplay between fission dynamics and the dominant vibrational mode.
The Journal of Chemical Physics
© 2017 American Institute of Physics. This paper was published in The Journal of Chemical Physics and is made available as an electronic reprint (preprint) with permission of American Institute of Physics. The published version is available at: [http://dx.doi.org/10.1063/1.4973981]. One print or electronic copy may be made for personal use only. Systematic or multiple reproduction, distribution to multiple locations via electronic or other means, duplication of any material in this paper for a fee or for commercial purposes, or modification of the content of the paper is prohibited and is subject to penalties under law.