Core-to-core X-ray emission spectra from Wannier based multiplet ligand field theory
Recent advances using Density Functional Theory (DFT) to augment Multiplet Ligand Field Theory (MLFT) have led to ab-initio calculations of many formerly empirical parameters. This development makes MLFT more predictive instead of interpretive, thus improving its value for studies of highly correlat...
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| Published in: | Journal of electron spectroscopy and related phenomena 2024-01, Vol.270 (C), p.147419, Article 147419 |
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| Main Authors: | , , , , |
| Format: | Article |
| Language: | eng |
| Subjects: | |
| Online Access: | Get full text |
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| Summary: | Recent advances using Density Functional Theory (DFT) to augment Multiplet Ligand Field Theory (MLFT) have led to ab-initio calculations of many formerly empirical parameters. This development makes MLFT more predictive instead of interpretive, thus improving its value for studies of highly correlated 3d, 4d, and f-electron systems. Synchrotron time is always at a premium, and tools that provide predictive capabilities have clear value when it comes to planning studies. Here, we develop a DFT + MLFT based approach for core-to-core Kα x-ray emission spectra (XES) and evaluate its performance for a range of transition metal systems. We find good agreement between theory and experiment, as well as the ability to capture key spectral trends related to spin and oxidation state. We also discuss limitations of the model in the context of the remaining free parameters and suggest directions forward.
•New development of ab initio treatment of deep core-to-core x-ray emission spectra.•Improved treatment of density functional theory combined with multiplet ligand field theory.•Demonstration of simplified one-step treatment with lower computational cost. |
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| ISSN: | 0368-2048 1873-2526 |