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

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 dynam...

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Main Authors: 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, Nicolas Bottin, Hazem Yousef, David von Stetten, Piotr Łaski, Radosław Kamiński, Katarzyna N. Jarzembska, Rachel F. Wallick, Till Stensitzki, Renske M. van der Veen, Henrike M. Müller-Werkmeister, Gábor Molnár, Dao Xiang, Christopher Milne, Maciej Lorenc, Yifeng Jiang
Format: Article
Language:English
Published: Nature Portfolio 2025-02-01
Series:Nature Communications
Online Access:https://doi.org/10.1038/s41467-025-57202-0
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author 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
Nicolas Bottin
Hazem Yousef
David von Stetten
Piotr Łaski
Radosław Kamiński
Katarzyna N. Jarzembska
Rachel F. Wallick
Till Stensitzki
Renske M. van der Veen
Henrike M. Müller-Werkmeister
Gábor Molnár
Dao Xiang
Christopher Milne
Maciej Lorenc
Yifeng Jiang
author_facet 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
Nicolas Bottin
Hazem Yousef
David von Stetten
Piotr Łaski
Radosław Kamiński
Katarzyna N. Jarzembska
Rachel F. Wallick
Till Stensitzki
Renske M. van der Veen
Henrike M. Müller-Werkmeister
Gábor Molnár
Dao Xiang
Christopher Milne
Maciej Lorenc
Yifeng Jiang
author_sort Doriana Vinci
collection DOAJ
description 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.
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spelling doaj-art-f0caab481aeb42e381f31107557a3f082025-08-20T02:01:38ZengNature PortfolioNature Communications2041-17232025-02-0116111210.1038/s41467-025-57202-0Capturing ultrafast molecular motions and lattice dynamics in spin crossover film using femtosecond diffraction methodsDoriana Vinci0Karl Ridier1Fengfeng Qi2Fernando Ardana-Lamas3Peter Zalden4Lai Chung Liu5Tobias Eklund6Mads Sielemann Jakobsen7Robin Schubert8Dmitry Khakhulin9Carsten Deiter10Nicolas Bottin11Hazem Yousef12David von Stetten13Piotr Łaski14Radosław Kamiński15Katarzyna N. Jarzembska16Rachel F. Wallick17Till Stensitzki18Renske M. van der Veen19Henrike M. Müller-Werkmeister20Gábor Molnár21Dao Xiang22Christopher Milne23Maciej Lorenc24Yifeng Jiang25European XFELLaboratoire de Chimie de Coordination, CNRS UPR 8241, Université de ToulouseKey Laboratory for Laser Plasmas (Ministry of Education), School of Physics and Astronomy, Shanghai Jiao Tong UniversityEuropean XFELEuropean XFELUncharted SoftwareEuropean XFELCenter for Data and Computing in Natural Sciences (CDCS)European XFELEuropean XFELEuropean XFELEuropean XFELEuropean XFELEuropean Molecular Biology Laboratory (EMBL), Hamburg unit c/o DESYUniversity of Warsaw, Faculty of ChemistryUniversity of Warsaw, Faculty of ChemistryUniversity of Warsaw, Faculty of ChemistryDepartment of Chemistry, University of Illinois Urbana-ChampaignInstitute of Chemistry, University of PotsdamDepartment of Chemistry, University of Illinois Urbana-ChampaignInstitute of Chemistry, University of PotsdamLaboratoire de Chimie de Coordination, CNRS UPR 8241, Université de ToulouseKey Laboratory for Laser Plasmas (Ministry of Education), School of Physics and Astronomy, Shanghai Jiao Tong UniversityEuropean XFELUniv. Rennes, CNRS, IPR (Institut de Physique de Rennes), UMR 6251European XFELAbstract 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.https://doi.org/10.1038/s41467-025-57202-0
spellingShingle 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
Nicolas Bottin
Hazem Yousef
David von Stetten
Piotr Łaski
Radosław Kamiński
Katarzyna N. Jarzembska
Rachel F. Wallick
Till Stensitzki
Renske M. van der Veen
Henrike M. Müller-Werkmeister
Gábor Molnár
Dao Xiang
Christopher Milne
Maciej Lorenc
Yifeng Jiang
Capturing ultrafast molecular motions and lattice dynamics in spin crossover film using femtosecond diffraction methods
Nature Communications
title Capturing ultrafast molecular motions and lattice dynamics in spin crossover film using femtosecond diffraction methods
title_full Capturing ultrafast molecular motions and lattice dynamics in spin crossover film using femtosecond diffraction methods
title_fullStr Capturing ultrafast molecular motions and lattice dynamics in spin crossover film using femtosecond diffraction methods
title_full_unstemmed Capturing ultrafast molecular motions and lattice dynamics in spin crossover film using femtosecond diffraction methods
title_short Capturing ultrafast molecular motions and lattice dynamics in spin crossover film using femtosecond diffraction methods
title_sort capturing ultrafast molecular motions and lattice dynamics in spin crossover film using femtosecond diffraction methods
url https://doi.org/10.1038/s41467-025-57202-0
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