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Direct observation of nuclear reorganization driven by ultrafast spin transitions

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 reorganizat...

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Autores principales: Jiang, Yifeng, Liu, Lai Chung, Sarracini, Antoine, Krawczyk, Kamil M., Wentzell, Jordan S., Lu, Cheng, Field, Ryan L., Matar, Samir F., Gawelda, Wojciech, Müller-Werkmeister, Henrike M., Miller, R. J. Dwayne
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group UK 2020
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC7090058/
https://www.ncbi.nlm.nih.gov/pubmed/32251278
http://dx.doi.org/10.1038/s41467-020-15187-y
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author Jiang, Yifeng
Liu, Lai Chung
Sarracini, Antoine
Krawczyk, Kamil M.
Wentzell, Jordan S.
Lu, Cheng
Field, Ryan L.
Matar, Samir F.
Gawelda, Wojciech
Müller-Werkmeister, Henrike M.
Miller, R. J. Dwayne
author_facet Jiang, Yifeng
Liu, Lai Chung
Sarracini, Antoine
Krawczyk, Kamil M.
Wentzell, Jordan S.
Lu, Cheng
Field, Ryan L.
Matar, Samir F.
Gawelda, Wojciech
Müller-Werkmeister, Henrike M.
Miller, R. J. Dwayne
author_sort Jiang, Yifeng
collection PubMed
description 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 [Fe(II)(bpy)(3)](PF(6))(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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spelling pubmed-70900582020-03-26 Direct observation of nuclear reorganization driven by ultrafast spin transitions Jiang, Yifeng Liu, Lai Chung Sarracini, Antoine Krawczyk, Kamil M. Wentzell, Jordan S. Lu, Cheng Field, Ryan L. Matar, Samir F. Gawelda, Wojciech Müller-Werkmeister, Henrike M. Miller, R. J. Dwayne Nat Commun Article 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 [Fe(II)(bpy)(3)](PF(6))(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. Nature Publishing Group UK 2020-03-23 /pmc/articles/PMC7090058/ /pubmed/32251278 http://dx.doi.org/10.1038/s41467-020-15187-y Text en © The Author(s) 2020 Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/.
spellingShingle Article
Jiang, Yifeng
Liu, Lai Chung
Sarracini, Antoine
Krawczyk, Kamil M.
Wentzell, Jordan S.
Lu, Cheng
Field, Ryan L.
Matar, Samir F.
Gawelda, Wojciech
Müller-Werkmeister, Henrike M.
Miller, R. J. Dwayne
Direct observation of nuclear reorganization driven by ultrafast spin transitions
title Direct observation of nuclear reorganization driven by ultrafast spin transitions
title_full Direct observation of nuclear reorganization driven by ultrafast spin transitions
title_fullStr Direct observation of nuclear reorganization driven by ultrafast spin transitions
title_full_unstemmed Direct observation of nuclear reorganization driven by ultrafast spin transitions
title_short Direct observation of nuclear reorganization driven by ultrafast spin transitions
title_sort direct observation of nuclear reorganization driven by ultrafast spin transitions
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC7090058/
https://www.ncbi.nlm.nih.gov/pubmed/32251278
http://dx.doi.org/10.1038/s41467-020-15187-y
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