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A molecular movie of ultrafast singlet fission

Author

Listed:
  • Christoph Schnedermann

    (University of Cambridge
    Oxford University)

  • Antonios M. Alvertis

    (University of Cambridge)

  • Torsten Wende

    (Oxford University)

  • Steven Lukman

    (University of Cambridge
    Agency for Science Technology and Research (A*STAR))

  • 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
    Cornell University, Baker Laboratory)

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.

Suggested Citation

  • 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 , 2019. "A molecular movie of ultrafast singlet fission," Nature Communications, Nature, vol. 10(1), pages 1-11, December.
    • Handle: RePEc:nat:natcom:v:10:y:2019:i:1:d:10.1038_s41467-019-12220-7
    DOI: 10.1038/s41467-019-12220-7
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    Cited by:

    1. Nilabja Maity & Woojae Kim & Naitik A. Panjwani & Arup Kundu & Kanad Majumder & Pranav Kasetty & Divji Mishra & Robert Bittl & Jayashree Nagesh & Jyotishman Dasgupta & Andrew J. Musser & Satish Patil, 2022. "Parallel triplet formation pathways in a singlet fission material," Nature Communications, Nature, vol. 13(1), pages 1-14, December.
    2. Stevens, Nicolas & Papavasiliou, Anthony, 2022. "Application of the Level Method for Computing Locational Convex Hull Prices," LIDAM Discussion Papers CORE 2022002, Université catholique de Louvain, Center for Operations Research and Econometrics (CORE).

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