Time-Resolved X-Ray Spectroscopy from the Atomic Orbital Ground State Up
X-ray spectroscopy has been a key method to determine ground- and excited-state properties of quantum materials with atomic specificity. Now, new x-ray facilities are opening the door to the study of pump-probe x-ray spectroscopy—specifically, time-resolved x-ray absorption (trXAS) and time-resolved...
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| Main Authors: | , , , , , , , , |
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| Format: | Article |
| Language: | English |
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American Physical Society
2025-01-01
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| Series: | Physical Review X |
| Online Access: | http://doi.org/10.1103/PhysRevX.15.011012 |
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| author | Daniel Jost Eder G. Lomeli Ta Tang Joshua J. Kas John J. Rehr Wei-Sheng Lee Hong-Chen Jiang Brian Moritz Thomas P. Devereaux |
| author_facet | Daniel Jost Eder G. Lomeli Ta Tang Joshua J. Kas John J. Rehr Wei-Sheng Lee Hong-Chen Jiang Brian Moritz Thomas P. Devereaux |
| author_sort | Daniel Jost |
| collection | DOAJ |
| description | X-ray spectroscopy has been a key method to determine ground- and excited-state properties of quantum materials with atomic specificity. Now, new x-ray facilities are opening the door to the study of pump-probe x-ray spectroscopy—specifically, time-resolved x-ray absorption (trXAS) and time-resolved resonant inelastic x-ray scattering (trRIXS). In this paper, we will present simulations of each of these spectroscopies using a time-domain full atomic multiplet, charge-transfer Hamiltonian adapted to study the properties of a generalized cluster model including a central transition-metal ion caged by ligand atoms in a planar geometry. The numerically evaluated trXAS and trRIXS cross sections for representative electron configurations 3d^{9} and 3d^{8} demonstrate the insights that can be obtained from charge-transfer pumping and how this nonequilibrium process affects ground- and excited-state properties. The straightforward characterization of the excitations in these systems based on our analysis of the simulations can serve as a benchmark for future experiments, as access to these time-resolved spectroscopic techniques becomes more widely available. |
| format | Article |
| id | doaj-art-8567d3b110e7463aa380532285c0cf4c |
| institution | Kabale University |
| issn | 2160-3308 |
| language | English |
| publishDate | 2025-01-01 |
| publisher | American Physical Society |
| record_format | Article |
| series | Physical Review X |
| spelling | doaj-art-8567d3b110e7463aa380532285c0cf4c2025-01-23T15:02:21ZengAmerican Physical SocietyPhysical Review X2160-33082025-01-0115101101210.1103/PhysRevX.15.011012Time-Resolved X-Ray Spectroscopy from the Atomic Orbital Ground State UpDaniel JostEder G. LomeliTa TangJoshua J. KasJohn J. RehrWei-Sheng LeeHong-Chen JiangBrian MoritzThomas P. DevereauxX-ray spectroscopy has been a key method to determine ground- and excited-state properties of quantum materials with atomic specificity. Now, new x-ray facilities are opening the door to the study of pump-probe x-ray spectroscopy—specifically, time-resolved x-ray absorption (trXAS) and time-resolved resonant inelastic x-ray scattering (trRIXS). In this paper, we will present simulations of each of these spectroscopies using a time-domain full atomic multiplet, charge-transfer Hamiltonian adapted to study the properties of a generalized cluster model including a central transition-metal ion caged by ligand atoms in a planar geometry. The numerically evaluated trXAS and trRIXS cross sections for representative electron configurations 3d^{9} and 3d^{8} demonstrate the insights that can be obtained from charge-transfer pumping and how this nonequilibrium process affects ground- and excited-state properties. The straightforward characterization of the excitations in these systems based on our analysis of the simulations can serve as a benchmark for future experiments, as access to these time-resolved spectroscopic techniques becomes more widely available.http://doi.org/10.1103/PhysRevX.15.011012 |
| spellingShingle | Daniel Jost Eder G. Lomeli Ta Tang Joshua J. Kas John J. Rehr Wei-Sheng Lee Hong-Chen Jiang Brian Moritz Thomas P. Devereaux Time-Resolved X-Ray Spectroscopy from the Atomic Orbital Ground State Up Physical Review X |
| title | Time-Resolved X-Ray Spectroscopy from the Atomic Orbital Ground State Up |
| title_full | Time-Resolved X-Ray Spectroscopy from the Atomic Orbital Ground State Up |
| title_fullStr | Time-Resolved X-Ray Spectroscopy from the Atomic Orbital Ground State Up |
| title_full_unstemmed | Time-Resolved X-Ray Spectroscopy from the Atomic Orbital Ground State Up |
| title_short | Time-Resolved X-Ray Spectroscopy from the Atomic Orbital Ground State Up |
| title_sort | time resolved x ray spectroscopy from the atomic orbital ground state up |
| url | http://doi.org/10.1103/PhysRevX.15.011012 |
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