IDEAS home Printed from https://ideas.repec.org/a/nat/natcom/v11y2020i1d10.1038_s41467-020-14468-w.html
   My bibliography  Save this article

Vibrational wavepacket dynamics in Fe carbene photosensitizer determined with femtosecond X-ray emission and scattering

Author

Listed:
  • Kristjan Kunnus

    (Stanford University)

  • Morgane Vacher

    (Uppsala University)

  • Tobias C. B. Harlang

    (Lund University
    Technical University of Denmark)

  • Kasper S. Kjær

    (Stanford University
    Lund University
    Technical University of Denmark)

  • Kristoffer Haldrup

    (Technical University of Denmark)

  • Elisa Biasin

    (Stanford University
    Technical University of Denmark)

  • Tim B. Driel

    (LCLS, SLAC National Accelerator Laboratory)

  • Mátyás Pápai

    (Technical University of Denmark)

  • Pavel Chabera

    (Lund University)

  • Yizhu Liu

    (Lund University
    Lund University)

  • Hideyuki Tatsuno

    (Lund University)

  • Cornelia Timm

    (Lund University)

  • Erik Källman

    (Uppsala University)

  • Mickaël Delcey

    (Uppsala University)

  • Robert W. Hartsock

    (Stanford University)

  • Marco E. Reinhard

    (Stanford University)

  • Sergey Koroidov

    (Stanford University)

  • Mads G. Laursen

    (Technical University of Denmark)

  • Frederik B. Hansen

    (Technical University of Denmark)

  • Peter Vester

    (Technical University of Denmark)

  • Morten Christensen

    (Technical University of Denmark)

  • Lise Sandberg

    (Technical University of Denmark
    University of Copenhagen, Niels Bohr Institute)

  • Zoltán Németh

    (Wigner Research Centre for Physics, Hungarian Academy of Sciences)

  • Dorottya Sárosiné Szemes

    (Wigner Research Centre for Physics, Hungarian Academy of Sciences)

  • Éva Bajnóczi

    (Wigner Research Centre for Physics, Hungarian Academy of Sciences)

  • Roberto Alonso-Mori

    (LCLS, SLAC National Accelerator Laboratory)

  • James M. Glownia

    (LCLS, SLAC National Accelerator Laboratory)

  • Silke Nelson

    (LCLS, SLAC National Accelerator Laboratory)

  • Marcin Sikorski

    (LCLS, SLAC National Accelerator Laboratory)

  • Dimosthenis Sokaras

    (SSRL, SLAC National Accelerator Laboratory)

  • Henrik T. Lemke

    (LCLS, SLAC National Accelerator Laboratory)

  • Sophie E. Canton

    (ELI-ALPS, ELI-HU Non-Profit Ltd.
    Deutsches Elektronen-Synchrotron (DESY))

  • Klaus B. Møller

    (Technical University of Denmark)

  • Martin M. Nielsen

    (Technical University of Denmark)

  • György Vankó

    (Wigner Research Centre for Physics, Hungarian Academy of Sciences)

  • Kenneth Wärnmark

    (Lund University)

  • Villy Sundström

    (Lund University)

  • Petter Persson

    (Lund University)

  • Marcus Lundberg

    (Uppsala University)

  • Jens Uhlig

    (Lund University)

  • Kelly J. Gaffney

    (Stanford University)

Abstract

The non-equilibrium dynamics of electrons and nuclei govern the function of photoactive materials. Disentangling these dynamics remains a critical goal for understanding photoactive materials. Here we investigate the photoinduced dynamics of the [Fe(bmip)2]2+ photosensitizer, where bmip = 2,6-bis(3-methyl-imidazole-1-ylidine)-pyridine, with simultaneous femtosecond-resolution Fe Kα and Kβ X-ray emission spectroscopy (XES) and X-ray solution scattering (XSS). This measurement shows temporal oscillations in the XES and XSS difference signals with the same 278 fs period oscillation. These oscillations originate from an Fe-ligand stretching vibrational wavepacket on a triplet metal-centered (3MC) excited state surface. This 3MC state is populated with a 110 fs time constant by 40% of the excited molecules while the rest relax to a 3MLCT excited state. The sensitivity of the Kα XES to molecular structure results from a 0.7% average Fe-ligand bond length shift between the 1 s and 2p core-ionized states surfaces.

Suggested Citation

  • Kristjan Kunnus & Morgane Vacher & Tobias C. B. Harlang & Kasper S. Kjær & Kristoffer Haldrup & Elisa Biasin & Tim B. Driel & Mátyás Pápai & Pavel Chabera & Yizhu Liu & Hideyuki Tatsuno & Cornelia Tim, 2020. "Vibrational wavepacket dynamics in Fe carbene photosensitizer determined with femtosecond X-ray emission and scattering," Nature Communications, Nature, vol. 11(1), pages 1-11, December.
    • Handle: RePEc:nat:natcom:v:11:y:2020:i:1:d:10.1038_s41467-020-14468-w
    DOI: 10.1038/s41467-020-14468-w
    as

    Download full text from publisher

    File URL: https://www.nature.com/articles/s41467-020-14468-w
    File Function: Abstract
    Download Restriction: no
    File URL: https://libkey.io/10.1038/s41467-020-14468-w?utm_source=ideas
    LibKey link: if access is restricted and if your library uses this service, LibKey will redirect you to where you can use your library subscription to access this item
    ---><---

    Citations

    Citations are extracted by the CitEc Project, subscribe to its RSS feed for this item.
    as


    Cited by:

    1. Robert B. Weakly & Chelsea E. Liekhus-Schmaltz & Benjamin I. Poulter & Elisa Biasin & Roberto Alonso-Mori & Andrew Aquila & Sébastien Boutet & Franklin D. Fuller & Phay J. Ho & Thomas Kroll & Caroline, 2023. "Revealing core-valence interactions in solution with femtosecond X-ray pump X-ray probe spectroscopy," Nature Communications, Nature, vol. 14(1), pages 1-8, December.
    2. Chia-Shuo Hsu & Jiali Wang & You-Chiuan Chu & Jui-Hsien Chen & Chia-Ying Chien & Kuo-Hsin Lin & Li Duan Tsai & Hsiao-Chien Chen & Yen-Fa Liao & Nozomu Hiraoka & Yuan-Chung Cheng & Hao Ming Chen, 2023. "Activating dynamic atomic-configuration for single-site electrocatalyst in electrochemical CO2 reduction," Nature Communications, Nature, vol. 14(1), pages 1-14, December.
    3. Marco Reinhard & Alessandro Gallo & Meiyuan Guo & Angel T. Garcia-Esparza & Elisa Biasin & Muhammad Qureshi & Alexander Britz & Kathryn Ledbetter & Kristjan Kunnus & Clemens Weninger & Tim Driel & Jos, 2023. "Ferricyanide photo-aquation pathway revealed by combined femtosecond Kβ main line and valence-to-core x-ray emission spectroscopy," Nature Communications, Nature, vol. 14(1), pages 1-11, December.

    More about this item

    Statistics

    Access and download statistics

    Corrections

    All material on this site has been provided by the respective publishers and authors. You can help correct errors and omissions. When requesting a correction, please mention this item's handle: RePEc:nat:natcom:v:11:y:2020:i:1:d:10.1038_s41467-020-14468-w. See general information about how to correct material in RePEc.

    If you have authored this item and are not yet registered with RePEc, we encourage you to do it here. This allows to link your profile to this item. It also allows you to accept potential citations to this item that we are uncertain about.

    We have no bibliographic references for this item. You can help adding them by using this form .

    If you know of missing items citing this one, you can help us creating those links by adding the relevant references in the same way as above, for each refering item. If you are a registered author of this item, you may also want to check the "citations" tab in your RePEc Author Service profile, as there may be some citations waiting for confirmation.

    For technical questions regarding this item, or to correct its authors, title, abstract, bibliographic or download information, contact: Sonal Shukla or Springer Nature Abstracting and Indexing (email available below). General contact details of provider: http://www.nature.com .

    Please note that corrections may take a couple of weeks to filter through the various RePEc services.

    IDEAS is a RePEc service. RePEc uses bibliographic data supplied by the respective publishers.