A molecular movie of ultrafast singlet fission

Christoph Schnedermann (), Antonios M. Alvertis, Torsten Wende, Steven Lukman, Jiaqi Feng, Florian A. Y. N. Schröder, David H. P. Turban, Jishan Wu, Nicholas D. M. Hine, Neil C. Greenham, Alex W. Chin, Akshay Rao, Philipp Kukura and Andrew J. Musser ()
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Christoph Schnedermann: University of Cambridge
Antonios M. Alvertis: University of Cambridge
Torsten Wende: Oxford University
Steven Lukman: University of Cambridge
Jiaqi Feng: National University of Singapore
Florian A. Y. N. Schröder: University of Cambridge
David H. P. Turban: University of Cambridge
Jishan Wu: National University of Singapore
Nicholas D. M. Hine: University of Warwick
Neil C. Greenham: University of Cambridge
Alex W. Chin: Institute des Nanosciences de Paris, Sorbonne Universite
Akshay Rao: University of Cambridge
Philipp Kukura: Oxford University
Andrew J. Musser: University of Sheffield

Nature Communications, 2019, vol. 10, issue 1, 1-11

Abstract: Abstract The complex dynamics of ultrafast photoinduced reactions are governed by their evolution along vibronically coupled potential energy surfaces. It is now often possible to identify such processes, but a detailed depiction of the crucial nuclear degrees of freedom involved typically remains elusive. Here, combining excited-state time-domain Raman spectroscopy and tree-tensor network state simulations, we construct the full 108-atom molecular movie of ultrafast singlet fission in a pentacene dimer, explicitly treating 252 vibrational modes on 5 electronic states. We assign the tuning and coupling modes, quantifying their relative intensities and contributions, and demonstrate how these modes coherently synchronise to drive the reaction. Our combined experimental and theoretical approach reveals the atomic-scale singlet fission mechanism and can be generalized to other ultrafast photoinduced reactions in complex systems. This will enable mechanistic insight on a detailed structural level, with the ultimate aim to rationally design molecules to maximise the efficiency of photoinduced reactions.

Date: 2019
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DOI: 10.1038/s41467-019-12220-7

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