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Capturing ultrafast molecular motions and lattice dynamics in spin crossover film using femtosecond diffraction methods

Author

Listed:
  • Doriana Vinci

    (European XFEL)

  • Karl Ridier

    (Université de Toulouse)

  • Fengfeng Qi

    (Shanghai Jiao Tong University)

  • Fernando Ardana-Lamas

    (European XFEL)

  • Peter Zalden

    (European XFEL)

  • Lai Chung Liu

    (Uncharted Software)

  • Tobias Eklund

    (European XFEL
    Condensed Matter Physics (KOMET), Institute of Physics, Johannes Gutenberg University Mainz)

  • Mads Sielemann Jakobsen

    (Center for Data and Computing in Natural Sciences (CDCS)
    Deutsches Elektronen-Synchrotron DESY)

  • Robin Schubert

    (European XFEL)

  • Dmitry Khakhulin

    (European XFEL)

  • Carsten Deiter

    (European XFEL)

  • Nicolas Bottin

    (European XFEL)

  • Hazem Yousef

    (European XFEL)

  • David Stetten

    (European Molecular Biology Laboratory (EMBL), Hamburg unit c/o DESY)

  • Piotr Łaski

    (University of Warsaw, Faculty of Chemistry)

  • Radosław Kamiński

    (University of Warsaw, Faculty of Chemistry)

  • Katarzyna N. Jarzembska

    (University of Warsaw, Faculty of Chemistry)

  • Rachel F. Wallick

    (Department of Chemistry, University of Illinois Urbana-Champaign)

  • Till Stensitzki

    (Institute of Chemistry, University of Potsdam)

  • Renske M. Veen

    (Department of Chemistry, University of Illinois Urbana-Champaign
    Helmholtz Zentrum Berlin für Materialien und Energie GmbH
    Institute of Optics and Atomic Physics, Technical University of Berlin)

  • Henrike M. Müller-Werkmeister

    (Institute of Chemistry, University of Potsdam)

  • Gábor Molnár

    (Université de Toulouse)

  • Dao Xiang

    (Shanghai Jiao Tong University
    Zhangjiang Institute for Advanced Study and Tsung-Dao Lee Institute, Shanghai Jiao Tong University)

  • Christopher Milne

    (European XFEL)

  • Maciej Lorenc

    (Univ. Rennes, CNRS, IPR (Institut de Physique de Rennes), UMR 6251
    CNRS, Univ Rennes, DYNACOM (Dynamical Control of Materials Laboratory), IRL2015, The University of Tokyo)

  • Yifeng Jiang

    (European XFEL)

Abstract

A comprehensive insight into ultrafast dynamics of photo-switchable materials is desired for efficient control of material properties through light excitation. Here, we study a polycrystalline spin crossover thin film as a prototypical example and reveal the sequential photo-switching dynamics, from local molecular rearrangement to global lattice deformation. On the earliest femtosecond timescale, the local molecular structural rearrangement occurs within a constant unit-cell volume through a two-step process, involving initial Fe−ligand bond elongation followed by ligand rotation. The highly-oriented structure of the nanocrystalline films and the experimental geometry enables resolving the full anisotropic lattice structural dynamics in and out of the sample plane separately. While both molecular switching and lattice heating influence lattice volume, they exert varying degrees of impact at disparate time scales following photoexcitation. This study highlights the opportunities provided by Mega-electron-volt electron and X-ray free electron laser to advance the understanding of ultrafast dynamics of photo-switchable materials.

Suggested Citation

  • Doriana Vinci & Karl Ridier & Fengfeng Qi & Fernando Ardana-Lamas & Peter Zalden & Lai Chung Liu & Tobias Eklund & Mads Sielemann Jakobsen & Robin Schubert & Dmitry Khakhulin & Carsten Deiter & Nicola, 2025. "Capturing ultrafast molecular motions and lattice dynamics in spin crossover film using femtosecond diffraction methods," Nature Communications, Nature, vol. 16(1), pages 1-12, December.
    • Handle: RePEc:nat:natcom:v:16:y:2025:i:1:d:10.1038_s41467-025-57202-0
    DOI: 10.1038/s41467-025-57202-0
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