English
 
User Manual Privacy Policy Disclaimer Contact us
  Advanced SearchBrowse

Item

ITEM ACTIONSEXPORT

Released

Journal Article

Intermolecular vibrations mediate ultrafast singlet fission

MPS-Authors
/persons/resource/persons136084

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;

/persons/resource/persons202750

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

/persons/resource/persons196471

Tiwari,  V.
Miller Group, Atomically Resolved Dynamics Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society;
Department of Chemistry, University of Hamburg;

/persons/resource/persons196491

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;

/persons/resource/persons136024

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 Ressource
Fulltext (public)

eabb0052.full.pdf
(Publisher version), 4MB

Supplementary Material (public)

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: http://hdl.handle.net/21.11116/0000-0006-EAA3-A
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.