Extreme Ultraviolet Reflection Spectroscopy of Lanthanides and Actinides Using a High Harmonic Generation Light Source.

Autor: Skrodzki PJ; Chemistry Division, Physical Chemistry and Applied Spectroscopy, Los Alamos National Laboratory, Los Alamos, New Mexico 87545, United States.; Center for Integrated Nanotechnologies, Los Alamos National Laboratory, Los Alamos, New Mexico 87545, United States., Livshits MY; Chemistry Division, Physical Chemistry and Applied Spectroscopy, Los Alamos National Laboratory, Los Alamos, New Mexico 87545, United States., Padmanabhan P; Center for Integrated Nanotechnologies, Los Alamos National Laboratory, Los Alamos, New Mexico 87545, United States., Greer SM; Chemistry Division, Physical Chemistry and Applied Spectroscopy, Los Alamos National Laboratory, Los Alamos, New Mexico 87545, United States., Buckway T; Chemistry Division, Physical Chemistry and Applied Spectroscopy, Los Alamos National Laboratory, Los Alamos, New Mexico 87545, United States.; Department of Physics and Astronomy, Brigham Young University, Provo, Utah 84602, United States., Elverson F; Chemistry Division, Physical Chemistry and Applied Spectroscopy, Los Alamos National Laboratory, Los Alamos, New Mexico 87545, United States., Gates C; Chemistry Division, Physical Chemistry and Applied Spectroscopy, Los Alamos National Laboratory, Los Alamos, New Mexico 87545, United States., Ward J; Chemistry Division, Physical Chemistry and Applied Spectroscopy, Los Alamos National Laboratory, Los Alamos, New Mexico 87545, United States., Roy P; Center for Integrated Nanotechnologies, Los Alamos National Laboratory, Los Alamos, New Mexico 87545, United States., Chen A; Center for Integrated Nanotechnologies, Los Alamos National Laboratory, Los Alamos, New Mexico 87545, United States., Sandberg RL; Department of Physics and Astronomy, Brigham Young University, Provo, Utah 84602, United States., Tretiak S; Center for Integrated Nanotechnologies, Los Alamos National Laboratory, Los Alamos, New Mexico 87545, United States.; Theoretical Division, Physics and Chemistry of Materials, Los Alamos National Laboratory, Los Alamos, New Mexico 87545, United States., Carpenter M; Nuclear Engineering and Nonproliferation, Safeguards, Science, and Technology, Los Alamos National Laboratory, Los Alamos, New Mexico 87545, United States., Stein B; Chemistry Division, Physical Chemistry and Applied Spectroscopy, Los Alamos National Laboratory, Los Alamos, New Mexico 87545, United States., Bowlan P; Chemistry Division, Physical Chemistry and Applied Spectroscopy, Los Alamos National Laboratory, Los Alamos, New Mexico 87545, United States.
Jazyk: angličtina
Zdroj: The journal of physical chemistry letters [J Phys Chem Lett] 2024 Jun 27; Vol. 15 (25), pp. 6544-6549. Date of Electronic Publication: 2024 Jun 17.
DOI: 10.1021/acs.jpclett.4c01051
Abstrakt: Absorption spectroscopy probing transitions from shallow-core d and f orbitals in lanthanides and actinides reveals information about bonding and the electronic structure in compounds containing these elements. However, spectroscopy in this photon energy range is challenging because of the limited availability of light sources and extremely short penetration depths. In this work, we address these challenges using a tabletop extreme ultraviolet (XUV), ultrafast, laser-driven, high harmonic generation light source, which generates femtosecond pulses in the 40-140 eV range. We present reflection spectroscopy measurements at the N 4,5 (i.e., predominantly 4d to 5f transitions) and O 4,5 (i.e., 5d to 5f transitions) absorption edges on several lanthanide and uranium oxide crystals. We compare these results to density functional theory calculations to assign the electronic transitions and predict the spectra for other lanthanides. This work paves the way for laboratory-scale XUV absorption experiments for studying crystalline and molecular f-electron systems, with applications ranging from surface chemistry, photochemistry, and electronic or chemical structure determination to nuclear forensics.
Databáze: MEDLINE
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