Non-Equilibrium Multiplet Excitations probed by the $M_{5,4}$ Branching Ratio in $3d \rightarrow 4f$ X-ray Absorption Spectroscopy
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arXiv
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| Autori principali: | , , , , , , , , |
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| Natura: | Preprint |
| Pubblicazione: |
2025
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| _version_ | 1866915262871109632 |
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| author | Amrhein, Tim Salantur, Beyza Püttner, Ralph Pontius, Niko Holldack, Karsten Wang, Ru-Pan Schüßler-Langeheine, Christian Weinelt, Martin Thielemann-Kühn, Nele |
| author_facet | Amrhein, Tim Salantur, Beyza Püttner, Ralph Pontius, Niko Holldack, Karsten Wang, Ru-Pan Schüßler-Langeheine, Christian Weinelt, Martin Thielemann-Kühn, Nele |
| contents | We show that ultrafast electronic $4f$ multiplet transitions in terbium metal are manifested by changes in the relative spectral weight of the $M_5$ and $M_4$ X-ray absorption resonances. Our experimental results are supported by a simulation of excited multiplet spectra with atomistic calculations; they prove that the so-called third rule of Thole and van der Laan, which relates the branching ratio of the spin-orbit split resonances to the total angular momentum $J$ of the excited ion, is also valid in non-equilibrium. The presented detection scheme allows to detect $J$-changing excitation, \textit{i.e}, alterations of spin and orbital states, even in samples without net magnetization. This makes branching-ratio spectroscopy a powerful tool for the quantitative investigation of ultrafast changes in angular momentum $J$. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2504_19630 |
| institution | arXiv |
| publishDate | 2025 |
| record_format | arxiv |
| spellingShingle | Non-Equilibrium Multiplet Excitations probed by the $M_{5,4}$ Branching Ratio in $3d \rightarrow 4f$ X-ray Absorption Spectroscopy Amrhein, Tim Salantur, Beyza Püttner, Ralph Pontius, Niko Holldack, Karsten Wang, Ru-Pan Schüßler-Langeheine, Christian Weinelt, Martin Thielemann-Kühn, Nele Materials Science Strongly Correlated Electrons We show that ultrafast electronic $4f$ multiplet transitions in terbium metal are manifested by changes in the relative spectral weight of the $M_5$ and $M_4$ X-ray absorption resonances. Our experimental results are supported by a simulation of excited multiplet spectra with atomistic calculations; they prove that the so-called third rule of Thole and van der Laan, which relates the branching ratio of the spin-orbit split resonances to the total angular momentum $J$ of the excited ion, is also valid in non-equilibrium. The presented detection scheme allows to detect $J$-changing excitation, \textit{i.e}, alterations of spin and orbital states, even in samples without net magnetization. This makes branching-ratio spectroscopy a powerful tool for the quantitative investigation of ultrafast changes in angular momentum $J$. |
| title | Non-Equilibrium Multiplet Excitations probed by the $M_{5,4}$ Branching Ratio in $3d \rightarrow 4f$ X-ray Absorption Spectroscopy |
| topic | Materials Science Strongly Correlated Electrons |
| url | https://arxiv.org/abs/2504.19630 |