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Ab Initio Prediction of Excited State and Polaron Effects in Transient XUV Measurements of α-Fe₂O₃

Klein, Isabel M. and Liu, Hanzhe and Nimlos, Danika and Krotz, Alex and Cushing, Scott K. (2022) Ab Initio Prediction of Excited State and Polaron Effects in Transient XUV Measurements of α-Fe₂O₃. . (Unpublished)

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Transient X-ray and extreme ultraviolet (XUV) spectroscopies have become invaluable tools for studying photoexcited dynamics due to their sensitivity to carrier occupations and local chemical or structural changes. One of the most studied mate-rials using transient XUV spectroscopy is α-Fe₂O₃ because of its rich photoexcited dynamics, including small polaron formation. The interpretation of carrier and polaron effects in α-Fe₂O₃ is currently done using a semi-empirical method that is not transferrable to most materials. Here, an ab initio, Bethe-Salpeter equation (BSE) approach is developed that can incorporate photoexcited state effects for arbitrary materials systems. The accuracy of this approach is proven by calculating the XUV absorption spectra for the ground, photoexcited, and polaron states of α-Fe₂O₃. Furthermore, the theoretical approach allows for the projection of the core-valence excitons and different components of the X-ray transition Hamiltonian onto the band structure, providing new insights into old measurements. From this information, a physical intuition about the origins and nature of the transient XUV spectra can be built. A route to extracting electron and hole energies is even shown possible for highly angular momentum split XUV peaks. This method is easily generalized to K, L, M, and N edges to provide a general approach for analyzing transient X-ray absorption or reflection data.

Item Type:Report or Paper (Discussion Paper)
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URLURL TypeDescription Paper
Liu, Hanzhe0000-0001-9001-725X
Nimlos, Danika0000-0002-5414-0039
Krotz, Alex0000-0001-8189-7902
Cushing, Scott K.0000-0003-3538-2259
Additional Information:Attribution-NonCommercial-NoDerivatives 4.0 International (CC BY-NC-ND 4.0).
Record Number:CaltechAUTHORS:20220517-214305241
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Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:114789
Deposited By: George Porter
Deposited On:18 May 2022 15:24
Last Modified:18 May 2022 15:24

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