Quantum-to-classical crossover in generalized spin systems: Temperature-dependent spin dynamics of FeI2

D. Dahlbom, F. T. Brooks, M. S. Wilson, S. Chi, A. I. Kolesnikov, M. B. Stone, H. Cao, Y. W. Li, K. Barros, M. Mourigal, C. D. Batista, X. Bai

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6 Scopus citations

Abstract

Simulating quantum spin systems at finite temperatures is an open challenge in many-body physics. This work studies the temperature-dependent spin dynamics of a pivotal compound, FeI2, to determine if universal quantum effects can be accounted for by a phenomenological renormalization of the dynamical spin structure factor S(q,ω) measured by inelastic neutron scattering. Renormalization schemes based on the quantum-to-classical correspondence principle are commonly applied at low temperatures to the harmonic oscillators describing normal modes. However, it is not clear how to extend this renormalization to arbitrarily high temperatures. Here we introduce a temperature-dependent normalization of the classical moments, the magnitude of which is determined by imposing the quantum sum rule, e.g., ∫dωdqS(q,ω)=NSS(S+1) for NS dipolar magnetic moments. We show that this simple renormalization scheme significantly improves the agreement between the calculated and measured S(q,ω) for FeI2 at all temperatures. Due to the coupled dynamics of dipolar and quadrupolar moments in that material, this renormalization procedure is extended to classical theories based on SU(3) coherent states, and by extension, to any SU(N) coherent state representation of local multipolar moments.

Original languageEnglish
Article number014427
JournalPhysical Review B
Volume109
Issue number1
DOIs
StatePublished - Jan 1 2024

Funding

The work of X.B. at LSU was supported by the Louisiana Board of Regents Support Fund. The work of K.B. was supported by the LANL LDRD program. The work of D.D. and C.D.B. at UTK, and F.TB., M.M., and X.B. (earlier work) at GT was supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences, and Engineering Division under Award No. DE-SC-0018660. We thank Tyrel McQueen and Adam Phelan for their help with crystal growth at the National Science Foundation's PARADIM (Platform for the Accelerated Realization, Analysis, and Discovery of Interface Materials), funded under Cooperative Agreement No. NSF-DMR-2039380. This research used resources at the High Flux Isotope Reactor and Spallation Neutron Source, a DOE Office of Science User Facility operated by the Oak Ridge National Laboratory.

FundersFunder number
LANL LDRD
National Science FoundationNSF-DMR-2039380
National Science Foundation
U.S. Department of Energy
Office of Science
Basic Energy Sciences
Louisiana Board of Regents
Division of Materials Sciences and EngineeringDE-SC-0018660
Division of Materials Sciences and Engineering

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