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High-pressure and magnetism in the quasi-one-dimensional solid solution Ca1−xNaxCr2O4: A multimodal neutron, muon, and x-ray study

E. Nocerino1,2,*, H. Sakurai3, O. K. Forslund4,5, K. Papadopoulos6, D. J. Mukkattukavil7, D. Andreica8, G. Simutis9, R. Khasanov9, N. Ishimatsu10 et al.

N. Kawamura11, C. L. Bull12,13, N. P. Funnell12, J. Sugiyama14, I. Umegaki15, Y. Sassa2, and M. Månsson2,†

  • *Contact author: elisabetta.nocerino@su.se
  • †Contact author: condmat@kth.se
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Phys. Rev. B 113, 104414 – Published 10 March, 2026

DOI: https://doi.org/10.1103/gpc2-fxmj

Abstract

We investigate the pressure-dependent magnetism of the quasi-one-dimensional solid solution Ca1−xNaxCr2O4 using neutron diffraction, Cr K-edge x-ray absorption spectroscopy, and muon spin rotation/relaxation. Na substitution is known to increase oxygen-ligand hole density (partial Cr3+ to Cr4+ character) and to drive the evolution from incommensurate order in CaCr2O4 to commensurate antiferromagnetism in NaCr2O4, suggesting a complex interplay between charge doping and structural changes. Here we apply hydrostatic pressure to tune the lattice without altering the nominal hole count, thereby separating compression effects from ligand-hole physics. For x=0 and x=0.5 the magnetic transition temperature is essentially pressure independent within our explored range, whereas in NaCr2O4 long-range order is progressively suppressed with pressure, as seen by a decrease of TN and of the magnetic Bragg intensity. Over the same pressure range, Cr K-edge x-ray absorption spectroscopy shows no resolvable change in the average Cr valence or coordination, and the refined corner-sharing Cr–O–Cr geometry remains nearly invariant within uncertainty. Extrapolating the pressure dependence of the magnetic order parameter suggests a critical pressure Pc=107(8) kbar for complete suppression of long-range order. These results support ligand-hole density as the primary control parameter across Ca1−xNaxCr2O4, with pressure acting as a secondary electronic tuning knob that weakens ordering in the Na-rich end member without inducing a new magnetic phase.

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Phys. Rev. B 113, 104414– Published 10 March, 2026
  • Received 5 May 2025
  • Revised 20 January 2026
  • Accepted 3 February 2026
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