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  Probing Transient Valence Orbital Changes with Picosecond Valence-to-Core X-ray Emission Spectroscopy

March, A. M., Assefa, T. A., Boemer, C., Bressler, C., Britz, A., Diez, M., et al. (2017). Probing Transient Valence Orbital Changes with Picosecond Valence-to-Core X-ray Emission Spectroscopy. The Journal of Physical Chemistry C, 121(5), 2620-2626. doi:10.1021/acs.jpcc.6b12940.

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Item Permalink: http://hdl.handle.net/11858/00-001M-0000-002D-7DAE-9 Version Permalink: http://hdl.handle.net/11858/00-001M-0000-002D-7DAF-7
Genre: Journal Article

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acs.jpcc.6b12940.pdf (Publisher version), 2MB
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2017
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© A. M. March
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https://doi.org/10.1021/acs.jpcc.6b12940 (Publisher version)
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 Creators:
March, Anne Marie1, Author
Assefa, Tadesse A.2, Author
Boemer, Christina2, 3, Author
Bressler, Christian2, 3, 4, Author
Britz, Alexander2, 3, 5, Author              
Diez, Michael2, 3, Author
Doumy, Gilles1, Author
Galler, Andreas2, Author
Harder, Manuel6, Author
Khakhulin, Dmitry2, 3, Author
Németh, Zoltán7, Author
Pápai, Mátyás7, 8, Author
Schulz, Sebastian2, 3, Author
Southworth, Stephen H.1, Author
Yavaş, Hasan6, Author
Young, Linda1, 9, Author
Gawelda, Wojciech2, 10, Author
Vankó, György7, Author
Affiliations:
1Chemical Sciences and Engineering Division, Argonne National Laboratory, Argonne, Illinois 60439, United States, ou_persistent22              
2European XFEL, Holzkoppel 4, D-22869 Schenefeld, Germany, ou_persistent22              
3The Hamburg Centre for Ultrafast Imaging, Luruper Chaussee 149, 22761 Hamburg, Germany, ou_persistent22              
4Department of Physics, Technical University of Denmark, Fysikvej 307, DK-2800, Kongens Lyngby, Denmark, ou_persistent22              
5International Max Planck Research School for Ultrafast Imaging & Structural Dynamics (IMPRS-UFAST), Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society, ou_2266714              
6Deutsches Elektronen-Synchrotron (DESY), 22607 Hamburg, Germany, ou_persistent22              
7Wigner Research Centre for Physics, Hungarian Academy Sciences, H-1525 Budapest, Hungary, ou_persistent22              
8Department of Chemistry, Technical University of Denmark, Kemitorvet 207, DK-2800, Kongens Lyngby, Denmark, ou_persistent22              
9Department of Physics and James Franck Institute, The University of Chicago, Chicago, Illinois 60637, United States, ou_persistent22              
10Institute of Physics, Jan Kochanowski University, 25-406 Kielce, Poland, ou_persistent22              

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 Abstract: We probe the dynamics of valence electrons in photoexcited [Fe(terpy)2]2+ in solution to gain deeper insight into the Fe–ligand bond changes. We use hard X-ray emission spectroscopy (XES), which combines element specificity and high penetration with sensitivity to orbital structure, making it a powerful technique for molecular studies in a wide variety of environments. A picosecond-time-resolved measurement of the complete 1s X-ray emission spectrum captures the transient photoinduced changes and includes the weak valence-to-core (vtc) emission lines that correspond to transitions from occupied valence orbitals to the nascent core-hole. Vtc-XES offers particular insight into the molecular orbitals directly involved in the light-driven dynamics; a change in the metal–ligand orbital overlap results in an intensity reduction and a blue energy shift in agreement with our theoretical calculations and more subtle features at the highest energies reflect changes in the frontier orbital populations.

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Language(s): eng - English
 Dates: 2016-10-232017-01-172017-02-09
 Publication Status: Published in print
 Pages: 7
 Publishing info: -
 Table of Contents: -
 Rev. Method: Peer
 Identifiers: DOI: 10.1021/acs.jpcc.6b12940
 Degree: -

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Title: The Journal of Physical Chemistry C
  Abbreviation : J. Phys. Chem. C
Source Genre: Journal
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Publ. Info: Washington, D.C. : American Chemical Society
Pages: - Volume / Issue: 121 (5) Sequence Number: - Start / End Page: 2620 - 2626 Identifier: ISSN: 1932-7447
CoNE: https://pure.mpg.de/cone/journals/resource/954926947766