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Spin-liquid-like ground states in the double hydroxyperovskites CuSn(OD)6 and MnSn(OD)6 evidenced by μSR spectroscopy

Moumita Naskar, Anton A. Kulbakov, Kaushick K. Parui, Jonas A. Krieger, Thomas J. Hicken, Hubertus Luetkens, Ellen Häußler, Thomas Doert, Darren C. Peets, Hans-Henning Klauss, Dmytro S. Inosov, Rajib Sarkar

Abstract

Double hydroxide perovskites with magnetic transition-metal ions were recently identified as a unique class of materials that combine magnetic frustration with correlated proton disorder-a prerequisite for quantum-disordered fluctuating magnetic ground states resembling spin liquids. Here we present the results of muon spin relaxation (μSR) measurements carried out on fully deuterated samples of the double hydroxyperovskites CuSn(OH)6 (S = 1/2) and MnSn(OH)6 (S = 5/2) over the temperature range 0.053-50 K. The absence of any long-range magnetic order is confirmed down to 0.053 K. We observe no oscillations of the muon asymmetry down to the lowest temperature. The muon relaxation rates show a continuous increase with decreasing temperature, indicating persistent spin fluctuations in both compounds. Spin correlations are consistent with homogeneous spin dynamics. These observations reinforce the assertion that both compounds have a quantum-dynamic magnetic ground state that is consistent with a spin-liquid-like phase stabilized by proton disorder.

Spin-liquid-like ground states in the double hydroxyperovskites CuSn(OD)6 and MnSn(OD)6 evidenced by μSR spectroscopy

Abstract

Double hydroxide perovskites with magnetic transition-metal ions were recently identified as a unique class of materials that combine magnetic frustration with correlated proton disorder-a prerequisite for quantum-disordered fluctuating magnetic ground states resembling spin liquids. Here we present the results of muon spin relaxation (μSR) measurements carried out on fully deuterated samples of the double hydroxyperovskites CuSn(OH)6 (S = 1/2) and MnSn(OH)6 (S = 5/2) over the temperature range 0.053-50 K. The absence of any long-range magnetic order is confirmed down to 0.053 K. We observe no oscillations of the muon asymmetry down to the lowest temperature. The muon relaxation rates show a continuous increase with decreasing temperature, indicating persistent spin fluctuations in both compounds. Spin correlations are consistent with homogeneous spin dynamics. These observations reinforce the assertion that both compounds have a quantum-dynamic magnetic ground state that is consistent with a spin-liquid-like phase stabilized by proton disorder.
Paper Structure (4 sections, 4 equations, 3 figures)

This paper contains 4 sections, 4 equations, 3 figures.

Table of Contents

  1. Introduction
  2. Experiment
  3. Results and discussion
  4. Conclusions

Figures (3)

  • Figure 1: Crystal structures of (a) CuSn(OD)$_6$ with orthorhombic $Pnnn$ symmetry Kulbakov2025a and (b) MnSn(OD)$_6$ with tetragonal $P4_2/n$ symmetry Parui2025. The Sn$^{4+}$-centered octahedra are shown in brown; the Cu$^{2+}$- and Mn$^{2+}$-centered octahedra in blue and green, respectively.
  • Figure 2: (a), (d) ZF-$\mu$SR time spectra measured at various temperatures for CuSn(OD)$_6$ and MnSn(OD)$_6$, respectively. Lines indicate the theoretical description as detailed in the text. (b), (c) Temperature dependencies of the width of the static field distribution and muon relaxation rate in zero-field $\mu$SR measurements of CuSn(OD)$_6$, respectively. (e), (f) Temperature evolution of the muon relaxation rates in ZF-$\mu$SR spectra of MnSn(OD)$_6$.
  • Figure 3: (a), (d) LF-$\mu$SR asymmetry spectra of CuSn(OD)$_6$ and MnSn(OD)$_6$ systems measured at 0.1 K. Lines correspond to the theoretical model discussed in the text. (b), (c) Field dependencies of the width of the static field distribution, muon relaxation rate in LF-$\mu$SR measurements of CuSn(OD)$_6$. (e), (f) Field evolution of the muon relaxation rates in LF-$\mu$SR spectra of MnSn(OD)$_6$.