Kondo quasiparticle dynamics observed by resonant inelastic x-ray scattering

M. C. Rahn; K. Kummer; A. Hariki; K. H. Ahn; J. Kuneš; A. Amorese; J. D. Denlinger; D. H. Lu; M. Hashimoto; E. Rienks; M. Valvidares; F. Haslbeck; D. D. Byler; K. J. McClellan; E. D. Bauer; J. X. Zhu; C. H. Booth; A. D. Christianson; J. M. Lawrence; F. Ronning; M. Janoschek

doi:10.1038/s41467-022-33468-6

Kondo quasiparticle dynamics observed by resonant inelastic x-ray scattering

M. C. Rahn, K. Kummer, A. Hariki, K. H. Ahn, J. Kuneš, A. Amorese, J. D. Denlinger, D. H. Lu, M. Hashimoto, E. Rienks, M. Valvidares, F. Haslbeck, D. D. Byler, K. J. McClellan, E. D. Bauer, J. X. Zhu, C. H. Booth, A. D. Christianson, J. M. Lawrence, F. RonningM. Janoschek

Correlated Electron Materials

Research output: Contribution to journal › Article › peer-review

7 Scopus citations

Abstract

Effective models focused on pertinent low-energy degrees of freedom have substantially contributed to our qualitative understanding of quantum materials. An iconic example, the Kondo model, was key to demonstrating that the rich phase diagrams of correlated metals originate from the interplay of localized and itinerant electrons. Modern electronic structure calculations suggest that to achieve quantitative material-specific models, accurate consideration of the crystal field and spin-orbit interactions is imperative. This poses the question of how local high-energy degrees of freedom become incorporated into a collective electronic state. Here, we use resonant inelastic x-ray scattering (RIXS) on CePd₃ to clarify the fate of all relevant energy scales. We find that even spin-orbit excited states acquire pronounced momentum-dependence at low temperature—the telltale sign of hybridization with the underlying metallic state. Our results demonstrate how localized electronic degrees of freedom endow correlated metals with new properties, which is critical for a microscopic understanding of superconducting, electronic nematic, and topological states.

Original language	English
Article number	6129
Journal	Nature Communications
Volume	13
Issue number	1
DOIs	https://doi.org/10.1038/s41467-022-33468-6
State	Published - Dec 2022

Funding

We are grateful for provision of experimental time at beamline ID32 of the European Synchrotron Radiation Facility (ESRF), Grenoble, France, at beamline BL5-2 of the Stanford Synchrotron Radiation Lightsource (SSRL) of the SLAC National Accelerator Laboratory, operated by the U.S. Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences (BES) under Contract No. DE-AC02-76SF00515, at beamline 4.0.3. of the Advanced Light Source, a U.S. DOE Office of Science User Facility under contract no. DE-AC02-05CH11231, at beamline UE112_PGM-2b-1^3 of the BESSY-II electron storage ring operated by the Helmholtz-Zentrum Berlin f\u00FCr Materialien und Energie (HZB), at beamline BL29 of the ALBA Synchrotron, Spain, and at the ARCS spectrometer at the Spallation Neutron Source, a DOE Office of Science User Facility operated by the Oak Ridge National Laboratory. Work at Los Alamos National Laboratory was performed under the auspices of the US Department of Energy, Office of Basic Energy Sciences, Division of Materials Sciences and Engineering. M.C.R. is grateful for support through the LANL Director\u2019s Fund and the Alexander von Humboldt Foundation. J.-X.Z. was supported by the Center for Integrated Nanotechnologies, a DOE BES user facility. J.K. was supported by the Fonds zur F\u00F6rderung der wissenschaftlichen Forschung (FWF) through QUAST-FOR5249 (project I 5868-N). A.H. was supported by JSPS KAKENHI Grant Number 21K13884 and\u00A021H01003. K.-H.A. was supported by the Czech Science Foundation Project Grant Number 19-06433S. A.D.C. was partially supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division. A.A. acknowledges the financial support of the Deutsche Forschungsgemeinschaft DFG under project SE1441/5-2. Work at TU Dresden was supported by the Deutsche Forschungsgemeinschaft through the CRC 1143 and the W\u00FCrzburg-Dresden Cluster of Excellence ct.qmat (EXC2147, Project ID 390858490). The work by F.H. and M.J. was supported through a Hans Fischer fellowship of the Technische Universit\u00E4t M\u00FCnchen-Institute for Advanced Study, funded by the German Excellence Initiative and the European Union Seventh Framework Programme under Grant agreement No. 291763. Special thanks are due to Daniel Mazzone, Johan Chang, Pascoal Pagliuso, Jason Hancock, and Peter Riseborough for insightful discussions. We are grateful for provision of experimental time at beamline ID32 of the European Synchrotron Radiation Facility (ESRF), Grenoble, France, at beamline BL5-2 of the Stanford Synchrotron Radiation Lightsource (SSRL) of the SLAC National Accelerator Laboratory, operated by the U.S. Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences (BES) under Contract No. DE-AC02-76SF00515, at beamline 4.0.3. of the Advanced Light Source, a U.S. DOE Office of Science User Facility under contract no. DE-AC02-05CH11231, at beamline UE112_PGM-2b-1^3 of the BESSY-II electron storage ring operated by the Helmholtz-Zentrum Berlin f\u00FCr Materialien und Energie (HZB), at beamline BL29 of the ALBA Synchrotron, Spain, and at the ARCS spectrometer at the Spallation Neutron Source, a DOE Office of Science User Facility operated by the Oak Ridge National Laboratory. Work at Los Alamos National Laboratory was performed under the auspices of the US Department of Energy, Office of Basic Energy Sciences, Division of Materials Sciences and Engineering. M.C.R. is grateful for support through the LANL Director\u2019s Fund and the Alexander von Humboldt Foundation. J.-X.Z. was supported by the Center for Integrated Nanotechnologies, a DOE BES user facility. J.K. was supported by the Fonds zur F\u00F6rderung der wissenschaftlichen Forschung (FWF) through QUAST-FOR5249 (project I 5868-N). A.H. was supported by JSPS KAKENHI Grant Number 21K13884 and 21H01003. K.-H.A. was supported by the Czech Science Foundation Project Grant Number 19-06433S. A.D.C. was partially supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division. A.A. acknowledges the financial support of the Deutsche Forschungsgemeinschaft DFG under project SE1441/5-2. Work at TU Dresden was supported by the Deutsche Forschungsgemeinschaft through the CRC 1143 and the W\u00FCrzburg-Dresden Cluster of Excellence ct.qmat (EXC2147, Project ID 390858490). The work by F.H. and M.J. was supported through a Hans Fischer fellowship of the Technische Universit\u00E4t M\u00FCnchen-Institute for Advanced Study, funded by the German Excellence Initiative and the European Union Seventh Framework Programme under Grant agreement No. 291763. Special thanks are due to Daniel Mazzone, Johan Chang, Pascoal Pagliuso, Jason Hancock, and Peter Riseborough for insightful discussions.

Funders	Funder number
Center for Integrated Nanotechnologies
Division of Materials Sciences and Engineering
Institute for Advanced Study, Technische Universität München
Oak Ridge National Laboratory
SLAC National Accelerator Laboratory
U.S. Department of Energy
German Excellence Initiative
Seventh Framework Programme
Helmholtz-Zentrum Berlin für Materialien und Energie
Alexander von Humboldt-Stiftung
Seventh Framework Programme	291763, 646807
Würzburg-Dresden Cluster of Excellence ct.qmat	EXC2147, 390858490
Basic Energy Sciences	DE-AC02-76SF00515
Grantová Agentura České Republiky	19-06433S
Japan Society for the Promotion of Science	21K13884, 21H01003
Office of Science	DE-AC02-05CH11231
Deutsche Forschungsgemeinschaft	CRC 1143, SE1441/5-2
Austrian Science Fund	I 5868-N, QUAST-FOR5249

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10.1038/s41467-022-33468-6

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Rahn, M. C., Kummer, K., Hariki, A., Ahn, K. H., Kuneš, J., Amorese, A., Denlinger, J. D., Lu, D. H., Hashimoto, M., Rienks, E., Valvidares, M., Haslbeck, F., Byler, D. D., McClellan, K. J., Bauer, E. D., Zhu, J. X., Booth, C. H., Christianson, A. D., Lawrence, J. M., ... Janoschek, M. (2022). Kondo quasiparticle dynamics observed by resonant inelastic x-ray scattering. Nature Communications, 13(1), Article 6129. https://doi.org/10.1038/s41467-022-33468-6

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title = "Kondo quasiparticle dynamics observed by resonant inelastic x-ray scattering",

abstract = "Effective models focused on pertinent low-energy degrees of freedom have substantially contributed to our qualitative understanding of quantum materials. An iconic example, the Kondo model, was key to demonstrating that the rich phase diagrams of correlated metals originate from the interplay of localized and itinerant electrons. Modern electronic structure calculations suggest that to achieve quantitative material-specific models, accurate consideration of the crystal field and spin-orbit interactions is imperative. This poses the question of how local high-energy degrees of freedom become incorporated into a collective electronic state. Here, we use resonant inelastic x-ray scattering (RIXS) on CePd3 to clarify the fate of all relevant energy scales. We find that even spin-orbit excited states acquire pronounced momentum-dependence at low temperature—the telltale sign of hybridization with the underlying metallic state. Our results demonstrate how localized electronic degrees of freedom endow correlated metals with new properties, which is critical for a microscopic understanding of superconducting, electronic nematic, and topological states.",

author = "Rahn, {M. C.} and K. Kummer and A. Hariki and Ahn, {K. H.} and J. Kune{\v s} and A. Amorese and Denlinger, {J. D.} and Lu, {D. H.} and M. Hashimoto and E. Rienks and M. Valvidares and F. Haslbeck and Byler, {D. D.} and McClellan, {K. J.} and Bauer, {E. D.} and Zhu, {J. X.} and Booth, {C. H.} and Christianson, {A. D.} and Lawrence, {J. M.} and F. Ronning and M. Janoschek",

note = "Publisher Copyright: {\textcopyright} 2022, The Author(s).",

year = "2022",

month = dec,

doi = "10.1038/s41467-022-33468-6",

language = "English",

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Rahn, MC, Kummer, K, Hariki, A, Ahn, KH, Kuneš, J, Amorese, A, Denlinger, JD, Lu, DH, Hashimoto, M, Rienks, E, Valvidares, M, Haslbeck, F, Byler, DD, McClellan, KJ, Bauer, ED, Zhu, JX, Booth, CH, Christianson, AD, Lawrence, JM, Ronning, F & Janoschek, M 2022, 'Kondo quasiparticle dynamics observed by resonant inelastic x-ray scattering', Nature Communications, vol. 13, no. 1, 6129. https://doi.org/10.1038/s41467-022-33468-6

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T1 - Kondo quasiparticle dynamics observed by resonant inelastic x-ray scattering

AU - Rahn, M. C.

AU - Kummer, K.

AU - Hariki, A.

AU - Ahn, K. H.

AU - Kuneš, J.

AU - Amorese, A.

AU - Denlinger, J. D.

AU - Lu, D. H.

AU - Hashimoto, M.

AU - Rienks, E.

AU - Valvidares, M.

AU - Haslbeck, F.

AU - Byler, D. D.

AU - McClellan, K. J.

AU - Bauer, E. D.

AU - Zhu, J. X.

AU - Booth, C. H.

AU - Christianson, A. D.

AU - Lawrence, J. M.

AU - Ronning, F.

AU - Janoschek, M.

PY - 2022/12

Y1 - 2022/12

N2 - Effective models focused on pertinent low-energy degrees of freedom have substantially contributed to our qualitative understanding of quantum materials. An iconic example, the Kondo model, was key to demonstrating that the rich phase diagrams of correlated metals originate from the interplay of localized and itinerant electrons. Modern electronic structure calculations suggest that to achieve quantitative material-specific models, accurate consideration of the crystal field and spin-orbit interactions is imperative. This poses the question of how local high-energy degrees of freedom become incorporated into a collective electronic state. Here, we use resonant inelastic x-ray scattering (RIXS) on CePd3 to clarify the fate of all relevant energy scales. We find that even spin-orbit excited states acquire pronounced momentum-dependence at low temperature—the telltale sign of hybridization with the underlying metallic state. Our results demonstrate how localized electronic degrees of freedom endow correlated metals with new properties, which is critical for a microscopic understanding of superconducting, electronic nematic, and topological states.

AB - Effective models focused on pertinent low-energy degrees of freedom have substantially contributed to our qualitative understanding of quantum materials. An iconic example, the Kondo model, was key to demonstrating that the rich phase diagrams of correlated metals originate from the interplay of localized and itinerant electrons. Modern electronic structure calculations suggest that to achieve quantitative material-specific models, accurate consideration of the crystal field and spin-orbit interactions is imperative. This poses the question of how local high-energy degrees of freedom become incorporated into a collective electronic state. Here, we use resonant inelastic x-ray scattering (RIXS) on CePd3 to clarify the fate of all relevant energy scales. We find that even spin-orbit excited states acquire pronounced momentum-dependence at low temperature—the telltale sign of hybridization with the underlying metallic state. Our results demonstrate how localized electronic degrees of freedom endow correlated metals with new properties, which is critical for a microscopic understanding of superconducting, electronic nematic, and topological states.

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Kondo quasiparticle dynamics observed by resonant inelastic x-ray scattering

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