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May 10, 2026Chemistry of Materials0 citations

Field-Induced Local Excitations Causing Zero-Magnetization Plateaus in Antiferromagnets of Antiferromagnetic Spin Dimers under Magnetic Field

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MWMyung-Hwan WhangboNorth Carolina State UniversityHKHyun-Joo KooKyung Hee UniversityNANikita V. AstakhovLomonosov Moscow State University

Key Points

  • This research investigates how magnetic fields influence the zero-magnetization plateau in antiferromagnetic spin dimers.
  • Analyzed energy spectrum of AFM chains composed of AFM spin dimers with S = 1/2 ions.
  • Examined magnetic entropy in the zero-magnetization plateaus across different field regions.
  • Conducted specific heat measurements for KCuCl3 at 2 K to validate theoretical predictions.
  • Field-induced local excitations successfully explain observations in TlCuCl3 and KCuCl3.
  • Identified two subregions of magnetic entropy within the field range from 0 to μ0Hc.
  • Verified specific heat field-dependence predictions for the two-phase region of the zero-magnetization plateau.

Abstract

The zero-magnetization plateau refers to the phenomenon that the magnetization of an antiferromagnet under a magnetic field remains at zero when the field increases from 0 to a certain critical value μ0Hc. Certain antiferromagnets composed of antiferromagnetic (AFM) spin dimers exhibit a zero-magnetization plateau despite the fact that the single-ion anisotropy of their magnetic ions is negligible. To investigate the cause for this finding, we analyzed how a magnetic field affects the energy spectrum of an AFM chain composed of AFM spin dimers made up of two S = 1/2 ions under the supposition that each spin dimer counteracts external field, according to Le Chatelier’s principle, to introduce a small amount of spin into the ground state (S = 0) by mixing the excited state (S = 1). First, we show that this concept of field-induced local excitations explains several puzzling observations concerning the zero-magnetization plateaus of TlCuCl3 and KCuCl3, which are antiferromagnets made up of molecular anions Cu2Cl62– (i.e., spin dimers of S = 1/2 ions Cu2+). Then, we analyze the magnetic entropy associated with the zero-magnetization plateaus occurring in the field region between 0 and μ0Hc to find that this field region is divided into two subregions of different magnetic entropy; the 0 – μ0Hm region where two different magnetic species coexist, the distribution of which in the spin–lattice generates the magnetic entropy described largely by the binomial coefficients, and the μ0Hm – μ0Hc region where there exists only one magnetic species, leading to zero magnetic entropy. We carried out specific heat measurements for KCuCl3 as a function of magnetic field between 0–9 T at 2 K and verified the predictions of our analysis concerning the field-dependence of specific heat for the two-phase region of a zero-magnetization plateau.

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Cite This Study

Whangbo et al. (2026) studied this question.

synapsesocial.com/papers/6a002222c8f74e3340f9d108https://doi.org/10.1021/acs.chemmater.6c00340
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