Evidence for spin liquid behavior in the frustrated three-dimensional <math xmlns="http://www.w3.org/1998/Math/MathML"><mrow><mi>S</mi><mo>=</mo><mn>1</mn><mo>/</mo><mn>2</mn></mrow></math> Heisenberg garnet <math xmlns="http://www.w3.org/1998/Math/MathML"><mrow><msub><mi>NaCa</mi><mn>2</mn></msub><msub><mi>Cu</mi><mn>2</mn></msub><msub><mrow><mo>(</mo><msub><mi>VO</mi><mn>4</mn></msub><mo>)</mo></mrow><mn>3</mn></msub></mrow></math>

Y. Alexanian; R. Kumar; H. Zeroual; B. Bernu; L. Mangin-Thro; J. R. Stewart; J. M. Wilkinson; S. Bhattacharya; P. L. Paulose; F. Bert; P. Mendels; B. Fåk; E. Kermarrec

doi:10.1103/crg9-9txm

Evidence for spin liquid behavior in the frustrated three-dimensional $S = 1 / 2$ Heisenberg garnet ${NaCa}_{2} {Cu}_{2} {({VO}_{4})}_{3}$

Y. Alexanian ^1,*,†, R. Kumar ², H. Zeroual ², B. Bernu ³, L. Mangin-Thro ¹, J. R. Stewart ⁴, J. M. Wilkinson ⁴, S. Bhattacharya², P. L. Paulose⁵ et al.

F. Bert ², P. Mendels ², B. Fåk¹, and E. Kermarrec ^2,‡

¹Institut Laue-Langevin, 71 Avenue des Martyrs, CS 20156, 38042 Grenoble Cedex 9, France
²Université Paris-Saclay, CNRS, Laboratoire de Physique des Solides, 91405 Orsay, France
³Sorbonne Université, CNRS, Laboratoire de Physique Théorique de la Matière Condensée, 75252 Paris Cedex 05, France
⁴ISIS Neutron and Muon Source, Rutherford Appleton Laboratory, Didcot OX11 0QX, United Kingdom
⁵Department of Condensed Matter Physics and Materials Science, TIFR, Mumbai 400 005, India

^*Contact author: yann.alexanian@unige.ch
^†Present address: Department of Quantum Matter Physics, University of Geneva, CH-1211 Geneva, Switzerland.
^‡Contact author: edwin.kermarrec@universite-paris-saclay.fr

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Phys. Rev. Materials 9, 074411 – Published 24 July, 2025

DOI: https://doi.org/10.1103/crg9-9txm

Abstract

Three-dimensional quantum spin liquids have remained elusive, hindered by reduced quantum fluctuations from larger lattice connectivity inherent to high-dimensional systems. Here, we investigate the remarkable persistence of dynamical short-range magnetic correlations in the nearly body-centered cubic garnet ${NaCa}_{2} {Cu}_{2} {({VO}_{4})}_{3}$ down to $T = 50 m K$ , two orders of magnitude below its Curie-Weiss temperature. Using a combination of neutron and muon spectroscopies plus numerical simulations, we demonstrate that a dynamical regime emerges, characterized by a dual response in the inelastic spectrum composed of short-live dispersive excitations and a quasielastic component. Strongly frustrated exchange interactions combined with subtle temperature-dependent Jahn-Teller spin-lattice effects are a plausible mechanism to explain the origin of this spin-liquid behavior.

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Evidence for spin liquid behavior in the frustrated three-dimensional $S = 1 / 2$ Heisenberg garnet ${NaCa}_{2} {Cu}_{2} {({VO}_{4})}_{3}$

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Evidence for spin liquid behavior in the frustrated three-dimensional S=1/2 Heisenberg garnet NaCa2Cu2(VO4)3

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Evidence for spin liquid behavior in the frustrated three-dimensional $S = 1 / 2$ Heisenberg garnet ${NaCa}_{2} {Cu}_{2} {({VO}_{4})}_{3}$