Imaging Singlet Fission using Angle-Resolved Photoemission

ORAL

Abstract

Zachary H. Withers1, Sergey Chernov1, Jin Bakalis1, Alice Kunin1, Michael G. White2, Gerd Schönhense3, and Thomas K. Allison1,2

1Department of Physics and Astronomy, Stony Brook University, Stony Brook, New York 11794, USA

2Department of Chemistry, Stony Brook University, Stony Brook, New York 11794, USA

3Johannes Gutenberg-Universität, Institut für Physik, D-55099 Mainz, Germany



Many organic semiconductors exhibit a process called singlet fission, where an initially excited singlet exciton splits into two triplet excitons. This process makes these molecular materials attractive candidates for photovoltaic applications due to the additional charge carriers. However, the intermediate states involved in singlet exciton fission remain highly debated. High-performance time- and angle-resolved photoemission (tr-ARPES) using the combination of MHz repetition-rate high-harmonic generation (HHG) and time-of-flight momentum microscopy can be used to image the molecular orbitals involved in singlet fission [1,2,3]. We present results on the optimization of crystalline pentacene thin films for photoemission and initial tr-ARPES results elucidating the correlated triplet-pair intermediate states.



References

1. C. Corder, et al., Struct. Dyn. 5, 054301 (2018).

2. A. Kunin, et al., Phys. Rev. Letts. 130, 046202 (2023).

3. Wallauer, et al., Science, 371, 1056-1059, (2021).

*DOE: DESC0022004, AFOSR: FA9550-20-1-0259, NSF: GRFP

Presenters

  • Zachary H Withers

    • Stony Brook University

Authors

  • Zachary H Withers

    • Stony Brook University
  • Sergii Chernov

    • Stony Brook University
  • Jin Bakalis

    • Stony Brook University (SUNY)
  • Alice Kunin

    • Stony Brook University (SUNY)
  • Michael G White

    • Stony Brook University
  • Gerd Schönhense

    • Johannes Gutenberg-Universität
  • Thomas K Allison

    • Stony Brook University (SUNY)