Structural Dynamics upon Photoexcitation in a Spin Crossover Crystal Probed with Femtosecond Electron Diffraction

Angewandte Chemie
Yifeng JiangR J Dwayne Miller

Abstract

Photoexcitation of spin crossover (SCO) complexes can trigger extensive electronic spin transitions and transformation of molecular structure. However, the precise nature of the associated ultrafast structural dynamics remains elusive, especially in the solid state. Here, we studied a single-crystal SCO material with femtosecond electron diffraction (FED). The unique capability of FED allows us to directly probe atomic motions and to track ultrafast structural changes within a crystal lattice. By monitoring the time-dependent changes of the Bragg reflections, we observed the formation of a photoinduced structure similar to the thermally induced high-spin state. The data and refinement calculations indicate the global structural reorganization within 2.3 ps, as the metal-ligand bond distribution narrows during intramolecular vibrational energy redistribution (IVR) driving the intermolecular rearrangement. Three independent dynamical group are identified to model the structural dynamics upon photoinduced SCO.

References

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Citations

Jul 4, 2018·Chemistry : a European Journal·Eric Collet, Marco Cammarata
May 14, 2019·Physical Chemistry Chemical Physics : PCCP·Lorena E RosalenyAlejandro Gaita-Ariño
Nov 11, 2019·The Journal of Chemical Physics·S ZerdaneE Collet
Apr 7, 2020·Nature Communications·Yifeng JiangR J Dwayne Miller
Nov 27, 2019·Angewandte Chemie·Kuppusamy Senthil Kumar, Mario Ruben
Apr 21, 2021·Physical Chemistry Chemical Physics : PCCP·Kyle Barlow, J Olof Johansson
Jun 27, 2021·Science Advances·Hélène SeilerHeinrich Schwoerer
Nov 1, 2017·The Journal of Physical Chemistry Letters·Xu DongMatvey V Fedin

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