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Ultrafast orbital tomography of a pentacene film using time-resolved momentum microscopy at a FEL

Author

Listed:
  • Kiana Baumgärtner

    (Julius-Maximilians-Universität Würzburg, Am Hubland
    Julius-Maximilians-Universität Würzburg, Am Hubland)

  • Marvin Reuner

    (Universität Hamburg)

  • Christian Metzger

    (Julius-Maximilians-Universität Würzburg, Am Hubland
    Julius-Maximilians-Universität Würzburg, Am Hubland)

  • Dmytro Kutnyakhov

    (Deutsches Elektronen-Synchrotron DESY)

  • Michael Heber

    (Deutsches Elektronen-Synchrotron DESY)

  • Federico Pressacco

    (Deutsches Elektronen-Synchrotron DESY)

  • Chul-Hee Min

    (Julius-Maximilians-Universität Würzburg, Am Hubland
    Christian-Albrechts-Universität zu Kiel)

  • Thiago R. F. Peixoto

    (Julius-Maximilians-Universität Würzburg, Am Hubland
    Deutsches Elektronen-Synchrotron DESY)

  • Mario Reiser

    (European X-Ray Free-Electron Laser Facility)

  • Chan Kim

    (European X-Ray Free-Electron Laser Facility)

  • Wei Lu

    (European X-Ray Free-Electron Laser Facility)

  • Roman Shayduk

    (European X-Ray Free-Electron Laser Facility)

  • Manuel Izquierdo

    (European X-Ray Free-Electron Laser Facility)

  • Günter Brenner

    (Deutsches Elektronen-Synchrotron DESY)

  • Friedrich Roth

    (TU Bergakademie Freiberg
    Center for Efficient High Temperature Processes and Materials Conversion (ZeHS), TU Bergakademie Freiberg)

  • Achim Schöll

    (Julius-Maximilians-Universität Würzburg, Am Hubland)

  • Serguei Molodtsov

    (European X-Ray Free-Electron Laser Facility
    TU Bergakademie Freiberg
    Center for Efficient High Temperature Processes and Materials Conversion (ZeHS), TU Bergakademie Freiberg)

  • Wilfried Wurth

    (Deutsches Elektronen-Synchrotron DESY
    Universität Hamburg
    The Hamburg Centre for Ultrafast Imaging (CUI))

  • Friedrich Reinert

    (Julius-Maximilians-Universität Würzburg, Am Hubland
    Julius-Maximilians-Universität Würzburg, Am Hubland)

  • Anders Madsen

    (European X-Ray Free-Electron Laser Facility)

  • Daria Popova-Gorelova

    (Universität Hamburg
    The Hamburg Centre for Ultrafast Imaging (CUI))

  • Markus Scholz

    (Deutsches Elektronen-Synchrotron DESY
    European X-Ray Free-Electron Laser Facility)

Abstract

Time-resolved momentum microscopy provides insight into the ultrafast interplay between structural and electronic dynamics. Here we extend orbital tomography into the time domain in combination with time-resolved momentum microscopy at a free-electron laser (FEL) to follow transient photoelectron momentum maps of excited states of a bilayer pentacene film on Ag(110). We use optical pump and FEL probe pulses by keeping FEL source conditions to minimize space charge effects and radiation damage. From the momentum microscopy signal, we obtain time-dependent momentum maps of the excited-state dynamics of both pentacene layers separately. In a combined experimental and theoretical study, we interpret the observed signal for the bottom layer as resulting from the charge redistribution between the molecule and the substrate induced by excitation. We identify that the dynamics of the top pentacene layer resembles excited-state molecular dynamics.

Suggested Citation

  • Kiana Baumgärtner & Marvin Reuner & Christian Metzger & Dmytro Kutnyakhov & Michael Heber & Federico Pressacco & Chul-Hee Min & Thiago R. F. Peixoto & Mario Reiser & Chan Kim & Wei Lu & Roman Shayduk , 2022. "Ultrafast orbital tomography of a pentacene film using time-resolved momentum microscopy at a FEL," Nature Communications, Nature, vol. 13(1), pages 1-7, December.
    • Handle: RePEc:nat:natcom:v:13:y:2022:i:1:d:10.1038_s41467-022-30404-6
    DOI: 10.1038/s41467-022-30404-6
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    References listed on IDEAS

    as
    1. Evangelos T. Karamatskos & Sebastian Raabe & Terry Mullins & Andrea Trabattoni & Philipp Stammer & Gildas Goldsztejn & Rasmus R. Johansen & Karol Długołecki & Henrik Stapelfeldt & Marc J. J. Vrakking , 2019. "Molecular movie of ultrafast coherent rotational dynamics of OCS," Nature Communications, Nature, vol. 10(1), pages 1-7, December.
    2. Cosmin I. Blaga & Junliang Xu & Anthony D. DiChiara & Emily Sistrunk & Kaikai Zhang & Pierre Agostini & Terry A. Miller & Louis F. DiMauro & C. D. Lin, 2012. "Imaging ultrafast molecular dynamics with laser-induced electron diffraction," Nature, Nature, vol. 483(7388), pages 194-197, March.
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