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Title: Elucidating ultrafast electron dynamics at surfaces using extreme ultraviolet (XUV) reflection–absorption spectroscopy

Abstract

Here we review the recent development of extreme ultraviolet reflection–absorption (XUV-RA) spectroscopy. This method combines the benefits of X-ray absorption spectroscopy, such as element, oxidation, and spin state specificity, with surface sensitivity and ultrafast time resolution, having a probe depth of only a few nm and an instrument response less than 100 fs. Using this technique we investigated the ultrafast electron dynamics at a hematite (α-Fe2O3) surface. Surface electron trapping and small polaron formation both occur in 660 fs following photoexcitation. These kinetics are independent of surface morphology indicating that electron trapping is not mediated by defects. Instead, small polaron formation is proposed as the likely driving force for surface electron trapping. We also show that in Fe2O3, Co3O4, and NiO, band gap excitation promotes electron transfer from O 2p valence band states to metal 3d conduction band states. In addition to detecting the photoexcited electron at the metal M2,3-edge, the valence band hole is directly observed as transient signal at the O L1-edge. The size of the resulting charge transfer exciton is on the order of a single metal–oxygen bond length. Spectral shifts at the O L1-edge correlate with metal–oxygen bond covalency, confirming the relationship between valence band hybridizationmore » and the overpotential for water oxidation. Furthermore, these examples demonstrate the unique ability to measure ultrafast electron dynamics with element and chemical state resolution using XUV-RA spectroscopy. Accordingly, this method is poised to play an important role to reveal chemical details of previously unseen surface electron dynamics.« less

Authors:
ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]
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  1. The Ohio State Univ., Columbus, OH (United States)
Publication Date:
Research Org.:
The Ohio State Univ., Columbus, OH (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division
OSTI Identifier:
1594152
Alternate Identifier(s):
OSTI ID: 1434139
Grant/Contract Number:  
SC0014051; FA9550-15-1-0204
Resource Type:
Accepted Manuscript
Journal Name:
ChemComm
Additional Journal Information:
Journal Volume: 54; Journal Issue: 34; Journal ID: ISSN 1359-7345
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND TECHNOLOGY

Citation Formats

Biswas, Somnath, Husek, Jakub, and Baker, L. Robert. Elucidating ultrafast electron dynamics at surfaces using extreme ultraviolet (XUV) reflection–absorption spectroscopy. United States: N. p., 2018. Web. doi:10.1039/c8cc01745j.
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Biswas, Somnath, Husek, Jakub, & Baker, L. Robert. Elucidating ultrafast electron dynamics at surfaces using extreme ultraviolet (XUV) reflection–absorption spectroscopy. United States. https://doi.org/10.1039/c8cc01745j
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Biswas, Somnath, Husek, Jakub, and Baker, L. Robert. Fri . "Elucidating ultrafast electron dynamics at surfaces using extreme ultraviolet (XUV) reflection–absorption spectroscopy". United States. https://doi.org/10.1039/c8cc01745j. https://www.osti.gov/servlets/purl/1594152.
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@article{osti_1594152,
title = {Elucidating ultrafast electron dynamics at surfaces using extreme ultraviolet (XUV) reflection–absorption spectroscopy},
author = {Biswas, Somnath and Husek, Jakub and Baker, L. Robert},
abstractNote = {Here we review the recent development of extreme ultraviolet reflection–absorption (XUV-RA) spectroscopy. This method combines the benefits of X-ray absorption spectroscopy, such as element, oxidation, and spin state specificity, with surface sensitivity and ultrafast time resolution, having a probe depth of only a few nm and an instrument response less than 100 fs. Using this technique we investigated the ultrafast electron dynamics at a hematite (α-Fe2O3) surface. Surface electron trapping and small polaron formation both occur in 660 fs following photoexcitation. These kinetics are independent of surface morphology indicating that electron trapping is not mediated by defects. Instead, small polaron formation is proposed as the likely driving force for surface electron trapping. We also show that in Fe2O3, Co3O4, and NiO, band gap excitation promotes electron transfer from O 2p valence band states to metal 3d conduction band states. In addition to detecting the photoexcited electron at the metal M2,3-edge, the valence band hole is directly observed as transient signal at the O L1-edge. The size of the resulting charge transfer exciton is on the order of a single metal–oxygen bond length. Spectral shifts at the O L1-edge correlate with metal–oxygen bond covalency, confirming the relationship between valence band hybridization and the overpotential for water oxidation. Furthermore, these examples demonstrate the unique ability to measure ultrafast electron dynamics with element and chemical state resolution using XUV-RA spectroscopy. Accordingly, this method is poised to play an important role to reveal chemical details of previously unseen surface electron dynamics.},
doi = {10.1039/c8cc01745j},
journal = {ChemComm},
number = 34,
volume = 54,
place = {United States},
year = {Fri Apr 06 00:00:00 EDT 2018},
month = {Fri Apr 06 00:00:00 EDT 2018}
}
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    Controlling polaron formation at hematite surfaces by molecular functionalization probed by XUV reflection-absorption spectroscopy
    journal, September 2019

    • Biswas, Somnath; Wallentine, Spencer; Bandaranayake, Savini
    • The Journal of Chemical Physics, Vol. 151, Issue 10
    • DOI: 10.1063/1.5115163

    Transient absorption spectroscopy using high harmonic generation: a review of ultrafast X-ray dynamics in molecules and solids
    journal, April 2019

    • Geneaux, Romain; Marroux, Hugo J. B.; Guggenmos, Alexander
    • Philosophical Transactions of the Royal Society A: Mathematical, Physical and Engineering Sciences, Vol. 377, Issue 2145
    • DOI: 10.1098/rsta.2017.0463

    Ultrafast Dynamics of Charge Transfer and Photochemical Reactions in Solar Energy Conversion
    journal, October 2018

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