Achieving Surface Sensitivity in Ultrafast XUV Spectroscopy: M2,3-Edge Reflection–Absorption of Transition Metal Oxides
Abstract
Ultrafast extreme ultraviolet (XUV) spectroscopy is a powerful tool for probing electronic structure and charge carrier dynamics in catalytic materials because of its elemental, oxidation, coordination, and electronic spin-state sensitivity. To extend the benefits of this technique to investigating charge carrier dynamics at surfaces, we have developed near grazing-angle XUV reflection–absorption (RA) spectroscopy. Because RA spectra probe both the real (i.e., reflection) and the imaginary (i.e., attenuation) parts of the refractive index, a general method is required to analyze RA spectra. Using semiempirical calculations, we demonstrate that XUV RA spectra of first row transition metal oxides retain the element and chemical state specificity of XUV absorption spectroscopy. Finally, we find that the imaginary part of the refractive index reports on the chemical state of the metal center, while the real part is additionally sensitive to the surface morphology of the material.
- Authors:
-
- 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; US Air Force Office of Scientific Research (AFOSR)
- OSTI Identifier:
- 1594147
- Grant/Contract Number:
- SC0014051; FA9550-15-1-0204
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Physical Chemistry. C
- Additional Journal Information:
- Journal Volume: 121; Journal Issue: 29; Journal ID: ISSN 1932-7447
- Publisher:
- American Chemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; oxides; surface morphology; optical properties; quantum mechanics materials
Citation Formats
Cirri, Anthony, Husek, Jakub, Biswas, Somnath, and Baker, L. Robert. Achieving Surface Sensitivity in Ultrafast XUV Spectroscopy: M2,3-Edge Reflection–Absorption of Transition Metal Oxides. United States: N. p., 2017.
Web. doi:10.1021/acs.jpcc.7b05127.
Cirri, Anthony, Husek, Jakub, Biswas, Somnath, & Baker, L. Robert. Achieving Surface Sensitivity in Ultrafast XUV Spectroscopy: M2,3-Edge Reflection–Absorption of Transition Metal Oxides. United States. https://doi.org/10.1021/acs.jpcc.7b05127
Cirri, Anthony, Husek, Jakub, Biswas, Somnath, and Baker, L. Robert. Wed .
"Achieving Surface Sensitivity in Ultrafast XUV Spectroscopy: M2,3-Edge Reflection–Absorption of Transition Metal Oxides". United States. https://doi.org/10.1021/acs.jpcc.7b05127. https://www.osti.gov/servlets/purl/1594147.
@article{osti_1594147,
title = {Achieving Surface Sensitivity in Ultrafast XUV Spectroscopy: M2,3-Edge Reflection–Absorption of Transition Metal Oxides},
author = {Cirri, Anthony and Husek, Jakub and Biswas, Somnath and Baker, L. Robert},
abstractNote = {Ultrafast extreme ultraviolet (XUV) spectroscopy is a powerful tool for probing electronic structure and charge carrier dynamics in catalytic materials because of its elemental, oxidation, coordination, and electronic spin-state sensitivity. To extend the benefits of this technique to investigating charge carrier dynamics at surfaces, we have developed near grazing-angle XUV reflection–absorption (RA) spectroscopy. Because RA spectra probe both the real (i.e., reflection) and the imaginary (i.e., attenuation) parts of the refractive index, a general method is required to analyze RA spectra. Using semiempirical calculations, we demonstrate that XUV RA spectra of first row transition metal oxides retain the element and chemical state specificity of XUV absorption spectroscopy. Finally, we find that the imaginary part of the refractive index reports on the chemical state of the metal center, while the real part is additionally sensitive to the surface morphology of the material.},
doi = {10.1021/acs.jpcc.7b05127},
journal = {Journal of Physical Chemistry. C},
number = 29,
volume = 121,
place = {United States},
year = {Wed Jun 28 00:00:00 EDT 2017},
month = {Wed Jun 28 00:00:00 EDT 2017}
}
Web of Science
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