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Disentangling the multiorbital contributions of excitons by photoemission exciton tomography

Author

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  • Wiebke Bennecke

    (Georg-August-Universität Göttingen)

  • Andreas Windischbacher

    (University of Graz, NAWI Graz)

  • David Schmitt

    (Georg-August-Universität Göttingen)

  • Jan Philipp Bange

    (Georg-August-Universität Göttingen)

  • Ralf Hemm

    (University of Kaiserslautern-Landau)

  • Christian S. Kern

    (University of Graz, NAWI Graz)

  • Gabriele D’Avino

    (Univ. Grenoble Alpes, CNRS, Inst NEEL)

  • Xavier Blase

    (Univ. Grenoble Alpes, CNRS, Inst NEEL)

  • Daniel Steil

    (Georg-August-Universität Göttingen)

  • Sabine Steil

    (Georg-August-Universität Göttingen)

  • Martin Aeschlimann

    (University of Kaiserslautern-Landau)

  • Benjamin Stadtmüller

    (University of Kaiserslautern-Landau)

  • Marcel Reutzel

    (Georg-August-Universität Göttingen)

  • Peter Puschnig

    (University of Graz, NAWI Graz)

  • G. S. Matthijs Jansen

    (Georg-August-Universität Göttingen)

  • Stefan Mathias

    (Georg-August-Universität Göttingen
    University of Göttingen)

Abstract

Excitons are realizations of a correlated many-particle wave function, specifically consisting of electrons and holes in an entangled state. Excitons occur widely in semiconductors and are dominant excitations in semiconducting organic and low-dimensional quantum materials. To efficiently harness the strong optical response and high tuneability of excitons in optoelectronics and in energy-transformation processes, access to the full wavefunction of the entangled state is critical, but has so far not been feasible. Here, we show how time-resolved photoemission momentum microscopy can be used to gain access to the entangled wavefunction and to unravel the exciton’s multiorbital electron and hole contributions. For the prototypical organic semiconductor buckminsterfullerene (C60), we exemplify the capabilities of exciton tomography and achieve unprecedented access to key properties of the entangled exciton state including localization, charge-transfer character, and ultrafast exciton formation and relaxation dynamics.

Suggested Citation

  • Wiebke Bennecke & Andreas Windischbacher & David Schmitt & Jan Philipp Bange & Ralf Hemm & Christian S. Kern & Gabriele D’Avino & Xavier Blase & Daniel Steil & Sabine Steil & Martin Aeschlimann & Benj, 2024. "Disentangling the multiorbital contributions of excitons by photoemission exciton tomography," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
    • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-45973-x
    DOI: 10.1038/s41467-024-45973-x
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    References listed on IDEAS

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    1. Ouri Karni & Elyse Barré & Vivek Pareek & Johnathan D. Georgaras & Michael K. L. Man & Chakradhar Sahoo & David R. Bacon & Xing Zhu & Henrique B. Ribeiro & Aidan L. O’Beirne & Jenny Hu & Abdullah Al-M, 2022. "Structure of the moiré exciton captured by imaging its electron and hole," Nature, Nature, vol. 603(7900), pages 247-252, March.
    2. David Schmitt & Jan Philipp Bange & Wiebke Bennecke & AbdulAziz AlMutairi & Giuseppe Meneghini & Kenji Watanabe & Takashi Taniguchi & Daniel Steil & D. Russell Luke & R. Thomas Weitz & Sabine Steil & , 2022. "Formation of moiré interlayer excitons in space and time," Nature, Nature, vol. 608(7923), pages 499-503, August.
    3. Elmar Mitterreiter & Bruno Schuler & Ana Micevic & Daniel Hernangómez-Pérez & Katja Barthelmi & Katherine A. Cochrane & Jonas Kiemle & Florian Sigger & Julian Klein & Edward Wong & Edward S. Barnard &, 2021. "The role of chalcogen vacancies for atomic defect emission in MoS2," Nature Communications, Nature, vol. 12(1), pages 1-8, December.
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