Coupled-cluster approach to vibronic effects in resonant inelastic x-ray scattering of quantum materials: Application to a $5d^1$ rhenium oxide
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| Format: | Preprint |
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2026
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| _version_ | 1866912941773684736 |
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| author | Matsuzaki, Teruki Chibotaru, Liviu F. Alessio, Maristella Iwahara, Naoya |
| author_facet | Matsuzaki, Teruki Chibotaru, Liviu F. Alessio, Maristella Iwahara, Naoya |
| contents | First-principles analysis of the spectroscopic signatures of correlated quantum materials poses significant challenges due to the interplay between spin-orbit and vibronic couplings, as well as the need to describe both dynamic and static electron correlation to reach decent accuracy. In this work, we apply the equation-of-motion coupled-cluster (EOM-CC) method to derive the spin-orbit-lattice entangled vibronic states and predict the Re $L_3$ edge resonant inelastic x-ray scattering (RIXS) spectra of Ba$_2$MgReO$_6$. The EOM-CC yields interaction parameters in close agreement with those extracted from RIXS spectra, with errors of less than 5\%. In particular, the EOM-CC method allowed us to determine the weak vibronic coupling to the $T_{2g}$ vibrations, which is difficult to address experimentally. The simulated spectra indicate that vibronic coupling to the $T_{2g}$ modes gives rise to a shoulder on the elastic peak. Going beyond the conventional treatment, which focuses solely on $E_g$ modes, we show that vibronic couplings to both $T_{2g}$ and $E_g$ modes are required to account for the fine structure of the RIXS spectra. This work demonstrates that the EOM-CC method is a powerful tool for accurately predicting the complex local states at metal sites and spectroscopic signatures of correlated insulating materials. |
| format | Preprint |
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arxiv_https___arxiv_org_abs_2603_03551 |
| institution | arXiv |
| publishDate | 2026 |
| record_format | arxiv |
| spellingShingle | Coupled-cluster approach to vibronic effects in resonant inelastic x-ray scattering of quantum materials: Application to a $5d^1$ rhenium oxide Matsuzaki, Teruki Chibotaru, Liviu F. Alessio, Maristella Iwahara, Naoya Strongly Correlated Electrons First-principles analysis of the spectroscopic signatures of correlated quantum materials poses significant challenges due to the interplay between spin-orbit and vibronic couplings, as well as the need to describe both dynamic and static electron correlation to reach decent accuracy. In this work, we apply the equation-of-motion coupled-cluster (EOM-CC) method to derive the spin-orbit-lattice entangled vibronic states and predict the Re $L_3$ edge resonant inelastic x-ray scattering (RIXS) spectra of Ba$_2$MgReO$_6$. The EOM-CC yields interaction parameters in close agreement with those extracted from RIXS spectra, with errors of less than 5\%. In particular, the EOM-CC method allowed us to determine the weak vibronic coupling to the $T_{2g}$ vibrations, which is difficult to address experimentally. The simulated spectra indicate that vibronic coupling to the $T_{2g}$ modes gives rise to a shoulder on the elastic peak. Going beyond the conventional treatment, which focuses solely on $E_g$ modes, we show that vibronic couplings to both $T_{2g}$ and $E_g$ modes are required to account for the fine structure of the RIXS spectra. This work demonstrates that the EOM-CC method is a powerful tool for accurately predicting the complex local states at metal sites and spectroscopic signatures of correlated insulating materials. |
| title | Coupled-cluster approach to vibronic effects in resonant inelastic x-ray scattering of quantum materials: Application to a $5d^1$ rhenium oxide |
| topic | Strongly Correlated Electrons |
| url | https://arxiv.org/abs/2603.03551 |