Microscopic origin of temperature-dependent magnetism in spin-orbit-coupled transition metal compounds

Li, Ying; Seshadri, Ram; Wilson, Stephen D.; Cheetham, Anthony K.; Valentí, Roser

doi:10.1103/PhysRevResearch.7.L012083

Title: Microscopic origin of temperature-dependent magnetism in spin-orbit-coupled transition metal compounds

Journal Article · 27 March 2025 · Physical Review Research

DOI: https://doi.org/10.1103/PhysRevResearch.7.L012083 · OSTI ID:2540153

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A few $4 d$ and $5 d$ transition metal compounds with various electron fillings were recently found to exhibit magnetic susceptibilities $χ$ and magnetic moments that deviate from the well-established Kotani model. This model has been considered for decades to be the canonical expression for descriing the temperature dependence of magnetism in systems with nonnegligible spin-orbit coupling effects. In this paper, we uncover the origin of such discrepancies and determine the applicability and limitations of the Kotani model by calculating the temperature dependence of the magnetic moments of a series of $4 d$ (Ru-based) and $5 d$ (W-based) systems at different electron fillings. For this purpose, we perform exact diagonalization of -derived relativistic multiorbital Hubbard models on finite clusters and compute their magnetic susceptibilities. Comparison with experimentally measured magnetic properties indicates that contributions such as a temperature-independent $χ_{0}$ background, crystal field effects, Coulomb and Hund's couplings, and intersite interactions—not included in the Kotani model—are especially crucial for correctly describing the temperature dependence of $χ$ and magnetic moments at various electron fillings in these systems. Based on our results, we propose a generalized approach beyond the Kotani model to accurately describe their magnetism. Published by the American Physical Society 2025

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Research Organization:: University of California, Santa Barbara, CA (United States)

Sponsoring Organization:: National Natural Science Foundation of China; National Science Foundation (NSF); USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0017752

OSTI ID:: 2540153

Journal Information:: Physical Review Research, Journal Name: Physical Review Research Journal Issue: 1 Vol. 7; ISSN PPRHAI; ISSN 2643-1564

Publisher:: American Physical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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