Direct observation of nuclear reorganization driven by ultrafast spin transitions

Yifeng Jiang, Lai Chung Liu, Antoine Sarracini, Kamil M. Krawczyk, Jordan S. Wentzell, Cheng Lu, Ryan L. Field, Samir F. Matar, Wojciech Gawelda, Henrike M. Müller-Werkmeister and R. J. Dwayne Miller ()
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Yifeng Jiang: Max Planck Institute for the Structure and Dynamics of Matter
Lai Chung Liu: University of Toronto
Antoine Sarracini: University of Toronto
Kamil M. Krawczyk: University of Toronto
Jordan S. Wentzell: University of Toronto
Cheng Lu: University of Toronto
Ryan L. Field: University of Toronto
Samir F. Matar: Lebanese German University
Wojciech Gawelda: European XFEL
Henrike M. Müller-Werkmeister: University of Potsdam
R. J. Dwayne Miller: Max Planck Institute for the Structure and Dynamics of Matter

Nature Communications, 2020, vol. 11, issue 1, 1-8

Abstract: Abstract One of the most basic molecular photophysical processes is that of spin transitions and intersystem crossing between excited states surfaces. The change in spin states affects the spatial distribution of electron density through the spin orbit coupling interaction. The subsequent nuclear reorganization reports on the full extent of the spin induced change in electron distribution, which can be treated similarly to intramolecular charge transfer with effective reaction coordinates depicting the spin transition. Here, single-crystal [FeII(bpy)3](PF6)2, a prototypical system for spin crossover (SCO) dynamics, is studied using ultrafast electron diffraction in the single-photon excitation regime. The photoinduced SCO dynamics are resolved, revealing two distinct processes with a (450 ± 20)-fs fast component and a (2.4 ± 0.4)-ps slow component. Using principal component analysis, we uncover the key structural modes, ultrafast Fe–N bond elongations coupled with ligand motions, that define the effective reaction coordinate to fully capture the relevant molecular reorganization.

Date: 2020
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DOI: 10.1038/s41467-020-15187-y

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