Intermolecular vibrations mediate ultrafast singlet fission

Duan, H.-G.; Jha, A.; Li, X.; Tiwari, V.; Ye, H.; Nayak, P. K.; Zhu, X.-L.; Li, Z.; Martinez, T. J.; Thorwart, M.; Miller, R. J. D.

doi:10.1126/sciadv.abb0052

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Journal Article

Intermolecular vibrations mediate ultrafast singlet fission

MPS-Authors

Duan, H.-G.
Miller Group, Atomically Resolved Dynamics Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society;
I. Institut für Theoretische Physik, Universität Hamburg;
The Hamburg Center for Ultrafast Imaging;

Jha, A.
Miller Group, Atomically Resolved Dynamics Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society;

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Tiwari, V.
Miller Group, Atomically Resolved Dynamics Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society;
International Max Planck Research School for Ultrafast Imaging & Structural Dynamics (IMPRS-UFAST), Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society;
Department of Chemistry, University of Hamburg;

Li, Z.
Miller Group, Atomically Resolved Dynamics Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society;
State Key Laboratory for Mesoscopic Physics, School of Physics, Peking University;

Miller, R. J. D.
Miller Group, Atomically Resolved Dynamics Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society;
The Hamburg Center for Ultrafast Imaging;
Departments of Chemistry and Physics, University of Toronto;

External Resource

https://arxiv.org/abs/1910.03338
(Preprint)

https://dx.doi.org/10.1126/sciadv.abb0052
(Publisher version)

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eabb0052.full.pdf
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abb0052_SM.pdf
(Supplementary material), 875KB

Citation

Duan, H.-G., Jha, A., Li, X., Tiwari, V., Ye, H., Nayak, P. K., et al. (2020). Intermolecular vibrations mediate ultrafast singlet fission. Science Advances, 6(38): eabb0052. doi:10.1126/sciadv.abb0052.

Cite as: https://hdl.handle.net/21.11116/0000-0007-0AA1-8

Abstract

Singlet fission is a spin-allowed exciton multiplication process in organic semiconductors that converts one spin-singlet exciton to two triplet excitons. It offers the potential to enhance solar energy conversion by circumventing the Shockley-Queisser limit on efficiency. We study the primary steps of singlet fission in a pentacene film by using a combination of TG and 2D electronic spectroscopy complemented by quantum chemical and nonadiabatic dynamics calculations. We show that the coherent vibrational dynamics induces the ultrafast transition from the singlet excited electronic state to the triplet-pair state via a degeneracy of potential energy surfaces, i.e., a multidimensional conical intersection. Significant vibronic coupling of the electronic wave packet to a few key intermolecular rocking modes in the low-frequency region connect the excited singlet and triplet-pair states. Along with high-frequency local vibrations acting as tuning modes, they open a new channel for the ultrafast exciton transfer through the resulting conical intersection.