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Random singlet physics in the S=12 pyrochlore antiferromagnet NaCdCu2F7

A. Kancko1, H. Sakai2, C. A. Corrêa3, P. Proschek1, J. Prokleška1, T. Haidamak1, M. Uhlarz4, A. Berlie5, Y. Tokunaga2 et al.

R. H. Colman1,*

  • *Contact author: ross.colman@matfyz.cuni.cz
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Phys. Rev. Research 8, 013344 – Published 31 March, 2026

DOI: https://doi.org/10.1103/rw5c-491w

Abstract

We report a random singlet ground state in the S=12 Heisenberg pyrochlore antiferromagnet NaCdCu2F7. Cationic Na+/Cd2+ disorder on the pyrochlore A site generates a broad distribution of Cu2+–F−–Cu2+ exchange couplings, introducing intrinsic magnetic bond disorder. Despite strong antiferromagnetic interactions (θCW=−72K), no magnetic order or global spin freezing is observed in dc and ac susceptibility, specific heat, or Na23 nuclear magnetic resonance to 120 mK, with muon spin relaxation experiments confirming persistent spin dynamics to 58 mK. T-linear specific heat, a Curie-like susceptibility tail, and power-law scaling with data collapse in χ(T), M(H), Cmag/T, Na23 (1/T1T), and the muon spin polarization P(t) reveal a disorder-driven network of random singlets and orphan spins. Scaling across multiple bulk and local probes is consistent with a broad distribution of exchange energies, P[J]∼J−α. This behavior contrasts with previously studied NaA″B2F7 pyrochlore fluorides, where magnetic bond disorder precipitates spin-glass freezing, underscoring the crucial role of strong S=12 quantum fluctuations in NaCdCu2F7.

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Phys. Rev. Research 8, 013344– Published 31 March, 2026
  • Received 24 September 2025
  • Accepted 9 March 2026
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