Phonons, Q -dependent Kondo spin fluctuations, and 4f phonon resonance in Yb Al3

Andrew D. Christianson, Victor R. Fanelli, Lucas Lindsay, Sai Mu, Marein C. Rahn, Daniel G. Mazzone, Ayman H. Said, Filip Ronning, Eric D. Bauer, Jon M. Lawrence

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2 Scopus citations

Abstract

4f intermediate valence (IV) compounds are canonical hosts of correlated electron physics and can contribute to our understanding of the larger class of correlated electron materials. Here we study the prototype IV compound YbAl3 which exhibits a nonintegral valence with a moderately heavy fermion ground state and a large Kondo temperature (TK∼500-600K). To better characterize the correlated physics of YbAl3, we have measured the phonon and the magnetic excitation spectra on single crystals of this material by time-of-flight inelastic neutron scattering and inelastic x-ray scattering. We have also performed theoretical calculations of the phonon spectra. We present three findings of these measurements. First, we observe that the measured phonon spectra can be described adequately by a calculation based on standard DFT+U density functional theory. The calculated energies, however, are 10% too low compared to the measured energies. This discrepancy may reflect a hardening of the phonons due to dynamic 4f correlations. Second, the low-temperature spin fluctuations on the Kondo energy scale kBTK have a momentum (Q) dependence similar to that seen recently in the IV compound CePd3. For that system, the Q dependence has been attributed to particle-hole excitations in a coherent itinerant 4f correlated ground state. We suggest a similar origin for the momentum dependence seen in YbAl3. This Q dependence disappears as the temperature is raised towards room temperature and the 4f electron band states become increasingly incoherent. Such a coherent/incoherent crossover is expected to be generic for correlated electron systems. Third, a low-temperature magnetic peak observed in the neutron scattering near 30 meV shows dispersion identical to a particular optic-phonon branch. This 4f/phonon resonance disappears for T≥150K. The phonon spectrum appears to be unaffected by the resonance. We discuss several possibilities for the origin of this unusual excitation, which may be unique to YbAl3. We suggest that the excitation may arise from the large amplitude beating of the light Al atoms against the heavy Yb atoms, resulting in a dynamic 4f/3p hybridization.

Original languageEnglish
Article number205135
JournalPhysical Review B
Volume102
Issue number20
DOIs
StatePublished - Nov 30 2020

Funding

Research at the Spallation Neutron Source at Oak Ridge National Laboratory was supported by the Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. Department of Energy (DOE). A.D.C. was supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division. During the early stages of this project A.D.C. was supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Scientific User Facilities Division. Density functional theory calculations were supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division. Work at LANL and the phonon calculations were supported by the U.S. DOE, Basic Energy Sciences, Division of Materials Science and Engineering. This research used resources of the Advanced Photon Source, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract No. DE-AC02-06CH11357. D.G.M. acknowledges support from the Swiss National Science Foundation, Fellowship No. P2EZP2_175092, and the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Science and Engineering Division, under Contract No. DE-SC0012704. M.C.R. is grateful for a postdoctoral fellowship by the Humboldt Society. This research has been supported by the Deutsche Forschungsgemeinschaft through the SFB 1143 and the Würzburg-Dresden Cluster of Excellence EXC 2147 (ct.qmat). We thank A. Banerjee and G. Sala for their assistance with the neutron-scattering measurements. This manuscript has been authored in part by UT-Battelle, LLC, under contract DE-AC05-00OR22725 with the U.S. Department of Energy (DOE). The U.S. government retains and the publisher, by accepting the article for publication, acknowledges that the U.S. government retains a nonexclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this manuscript, or allow others to do so, for U.S. government purposes.

FundersFunder number
Division of Materials Science and Engineering
Humboldt Society
Materials Science and Engineering DivisionDE-SC0012704
Office of Basic Energy Sciences
Scientific User Facilities Division
U.S. Department of Energy
Office of Science
Basic Energy Sciences
Argonne National LaboratoryDE-AC02-06CH11357
Los Alamos National Laboratory
Division of Materials Sciences and Engineering
Deutsche ForschungsgemeinschaftDE-AC05-00OR22725, EXC 2147, SFB 1143
Schweizerischer Nationalfonds zur Förderung der Wissenschaftlichen ForschungP2EZP2_175092

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