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  Direct observation of nuclear reorganization driven by ultrafast spin transitions

Jiang, Y., Liu, L. C., Sarracini, A., Krawczyk, K. M., Wentzell, J. S., Lu, C., et al. (2020). Direct observation of nuclear reorganization driven by ultrafast spin transitions. Nature Communications, 11(1): 1530. doi:10.1038/s41467-020-15187-y.

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Jiang, Y.1, Autor           
Liu, L. C.2, Autor
Sarracini, A.2, Autor
Krawczyk, K. M.2, Autor
Wentzell, J. S.2, Autor
Lu, C.2, Autor
Field, E. L.2, Autor
Matar, S. F.3, Autor
Gawelda, W.4, 5, Autor
Müller-Werkmeister, H. M.6, Autor
Miller, R. J. D.1, 2, Autor           
Affiliations:
1Miller Group, Atomically Resolved Dynamics Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society, ou_1938288              
2Departments of Chemistry and Physics, University of Toronto, ou_persistent22              
3Lebanese German University, LGU, Sahel-Alma Campus, ou_persistent22              
4European XFEL, ou_persistent22              
5Faculty of Physics, Adam Mickiewicz University, ou_persistent22              
6Institute of Chemistry, University of Potsdam, ou_persistent22              

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 Zusammenfassung: 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.

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Sprache(n): eng - English
 Datum: 2019-07-032020-02-112020-03-23
 Publikationsstatus: Online veröffentlicht
 Seiten: -
 Ort, Verlag, Ausgabe: -
 Inhaltsverzeichnis: -
 Art der Begutachtung: Expertenbegutachtung
 Identifikatoren: DOI: 10.1038/s41467-020-15187-y
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Grant ID : 623994
Förderprogramm : Funding Programme 7 (FP7)
Förderorganisation : European Commission (EC)

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Titel: Nature Communications
  Kurztitel : Nat. Commun.
Genre der Quelle: Zeitschrift
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Ort, Verlag, Ausgabe: London : Nature Publishing Group
Seiten: - Band / Heft: 11 (1) Artikelnummer: 1530 Start- / Endseite: - Identifikator: ISSN: 2041-1723
CoNE: https://pure.mpg.de/cone/journals/resource/2041-1723