Cited by 88X-ray Spectroscopy and Fluorescence AnalysisAdvanced X-ray Imaging TechniquesPhotochemistry and Electron Transfer Studies

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Excited-state molecular structures captured by X-ray transient absorption spectroscopy: a decade and beyond

Chen, Lin X., Zhang, Xiaoyi, Lockard, Jenny V., Stickrath, Andrew B., Attenkofer, Klaus, Jennings, Guy, Liu, Di-Jia·2010·Acta Crystallographica Section A Foundations of Crystallography

DOI 10.1107/s0108767309051496

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Abstract

Transient molecular structures along chemical reaction pathways are important for predicting molecular reactivity, understanding reaction mechanisms, as well as controlling reaction pathways. During the past decade, X-ray transient absorption spectroscopy (XTA, or LITR-XAS, laser-initiated X-ray absorption spectroscopy), analogous to the commonly used optical transient absorption spectroscopy, has been developed. XTA uses a laser pulse to trigger a fundamental chemical process, and an X-ray pulse(s) to probe transient structures as a function of the time delay between the pump and probe pulses. Using X-ray pulses with high photon flux from synchrotron sources, transient electronic and molecular structures of metal complexes have been studied in disordered media from homogeneous solutions to heterogeneous solution–solid interfaces. Several examples from the studies at the Advanced Photon Source in Argonne National Laboratory are summarized, including excited-state metalloporphyrins, metal-to-ligand charge transfer (MLCT) states of transition metal complexes, and charge transfer states of metal complexes at the interface with semiconductor nanoparticles. Recent developments of the method are briefly described followed by a future prospective of XTA. It is envisioned that concurrent developments in X-ray free-electron lasers and synchrotron X-ray facilities as well as other table-top laser-driven femtosecond X-ray sources will make many breakthroughs and realise dreams of visualizing molecular movies and snapshots, which ultimately enable chemical reaction pathways to be controlled.

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See all 88

Authors: Chen, L. X., Zhang, X., Lockard, J. V., Stickrath, A. B., Attenkofer, K., Jennings, G., & Liu, D.-J.
Affiliations: Northwestern University (US)
Argonne National Laboratory (US)
ORCID: Chen, Lin X.
Zhang, Xiaoyi
Lockard, Jenny V.
Attenkofer, Klaus
Jennings, Guy
Liu, Di-Jia
Venue: Acta Crystallographica Section A Foundations of Crystallography
Publisher: International Union of Crystallography (IUCr)
Published: 2010-02-18
Volume: 66
Issue: 2
Pages: 240-251
ISSN: 0108-7673 (ISSN-L)
DOI: 10.1107/s0108767309051496
OpenAlex: W2093910216
Cited by: 88
References: 111
Citations by year: 2026: 1 · 2024: 5 · 2023: 2 · 2022: 4 · 2021: 4 · 2020: 2 · 2019: 5 · 2018: 6 · 2017: 10 · 2016: 9 · 2015: 11 · 2014: 8 · 2013: 11 · 2012: 4
FWCI: 6.42
Type: journal article
Language: en
Open access: closed
Licence: journals.iucr.org/services/copyrightpolicy.html (vor)
journals.iucr.org/services/copyrightpolicy.html#TDM (tdm)
Locations: Acta Crystallographica Section A Foundations of Crystallography (publishedVersion)
PubMed (publishedVersion)
Topics: Physical Sciences › Physics and Astronomy › Radiation › X-ray Spectroscopy and Fluorescence Analysis
Physical Sciences › Physics and Astronomy › Radiation › Advanced X-ray Imaging Techniques
Physical Sciences › Chemistry › Physical and Theoretical Chemistry › Photochemistry and Electron Transfer Studies
Keywords: excited-state molecular structure, metalloporphyrins, metal-to-ligand charge transfer, transition metal complexes, reaction mechanism, femtosecond X-ray sources, X-ray free-electron laser, solid-solution interface

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Excited-state molecular structures captured by X-ray transient absorption spectroscopy: a decade and beyond

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