Crystal field excitations in rattling clathrate CeBa$_7$Au$_6$Si$_{40}$

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Main Authors: Tagliavini, Michelangelo, Mazza, Federico, Yan, Xinlin, Sidorenko, Andrey, Ackermann, Kevin, Prokofiev, Andrey, Kummer, Kurt, Paschen, Silke, Haverkort, Maurits W.
Format: Preprint
Published: 2025
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author Tagliavini, Michelangelo
Mazza, Federico
Yan, Xinlin
Sidorenko, Andrey
Ackermann, Kevin
Prokofiev, Andrey
Kummer, Kurt
Paschen, Silke
Haverkort, Maurits W.
author_facet Tagliavini, Michelangelo
Mazza, Federico
Yan, Xinlin
Sidorenko, Andrey
Ackermann, Kevin
Prokofiev, Andrey
Kummer, Kurt
Paschen, Silke
Haverkort, Maurits W.
contents We investigate the local crystal-field environment of cerium in the clathrate compound CeBa$_7$Au$_6$Si$_{40}$ (Ce-BAS) using resonant inelastic x-ray scattering (RIXS) and magnetic susceptibility measurements. Ce-BAS is a rare example of a system where heavy-fermion physics coexists with low-energy rattling phonon modes, making it a candidate for enhanced thermoelectric performance. Magnetic susceptibility measurements reveal a temperature-dependent local moment that cannot be explained within a static crystal-field model. A fit to the susceptibility data requires strong mixing between the j = 5/2 and j = 7/2 crystal-field states, which implies large internal splittings inconsistent with RIXS spectra. In contrast, RIXS data are well described by a model with negligible j = 5/2 - j = 7/2 mixing and an energy separation of 12 meV between the ground and first excited crystal-field states. The inability to reconcile these two datasets within a static framework points to a dynamical modification of the crystal-field potential. We attribute this to coupling between the Ce 4f electrons and low-energy phonons associated with the Ce rattling motion. This interpretation is consistent with theoretical predictions of phonon-enhanced Kondo effects and dynamical Jahn-Teller distortions. Our results highlight the need for multi-orbital impurity models that include phonon coupling to fully describe the low-energy physics of Ce-BAS.
format Preprint
id arxiv_https___arxiv_org_abs_2504_19802
institution arXiv
publishDate 2025
record_format arxiv
spellingShingle Crystal field excitations in rattling clathrate CeBa$_7$Au$_6$Si$_{40}$
Tagliavini, Michelangelo
Mazza, Federico
Yan, Xinlin
Sidorenko, Andrey
Ackermann, Kevin
Prokofiev, Andrey
Kummer, Kurt
Paschen, Silke
Haverkort, Maurits W.
Strongly Correlated Electrons
We investigate the local crystal-field environment of cerium in the clathrate compound CeBa$_7$Au$_6$Si$_{40}$ (Ce-BAS) using resonant inelastic x-ray scattering (RIXS) and magnetic susceptibility measurements. Ce-BAS is a rare example of a system where heavy-fermion physics coexists with low-energy rattling phonon modes, making it a candidate for enhanced thermoelectric performance. Magnetic susceptibility measurements reveal a temperature-dependent local moment that cannot be explained within a static crystal-field model. A fit to the susceptibility data requires strong mixing between the j = 5/2 and j = 7/2 crystal-field states, which implies large internal splittings inconsistent with RIXS spectra. In contrast, RIXS data are well described by a model with negligible j = 5/2 - j = 7/2 mixing and an energy separation of 12 meV between the ground and first excited crystal-field states. The inability to reconcile these two datasets within a static framework points to a dynamical modification of the crystal-field potential. We attribute this to coupling between the Ce 4f electrons and low-energy phonons associated with the Ce rattling motion. This interpretation is consistent with theoretical predictions of phonon-enhanced Kondo effects and dynamical Jahn-Teller distortions. Our results highlight the need for multi-orbital impurity models that include phonon coupling to fully describe the low-energy physics of Ce-BAS.
title Crystal field excitations in rattling clathrate CeBa$_7$Au$_6$Si$_{40}$
topic Strongly Correlated Electrons
url https://arxiv.org/abs/2504.19802