Unusually large magnetic moment and tricritical behavior of the CMR compound NaCr₂O₄ revealed with high resolution neutron diffraction and μ+ SR

Abstract The mixed valence Cr³⁺/Cr⁴⁺ compound NaCr₂O₄, hosts a plethora of unconventional electronic properties. In the present study, muon spin rotation/relaxation ( μ + SR) and high-resolution time-of-flight neutron powder diffraction measurements were carried out on high-quality samples to clarify the complex magnetic ground state of this unique material. We identified a commensurate canted antiferromagnetic order (C-AFM) with a canting angle of the Cr spin axial vector equal to θ c = ( 8.8 ± 0.5 ) ∘ , and an estimated Cr moment μ C r C ∼ ( 4.30 ± 0.01 ) μ B . Such an unusually large value of μ C r C is compatible with the existence of high-spin Cr sites created by the presence of an unconventional negative charge transfer state in NaCr₂O₄. In addition to the C-AFM structure, a novel magnetic supercell was also revealed. Such supercell display an incommensurate (IC)-AFM propagation vector (0 0 1 2 − δ ), having a Cr moment μ C r I C = ( 2.20 ± 0.03 ) μ B . It is suggested that the C-AFM and IC-AFM modulations have two different electronic origins, being due to itinerant and localized contributions to the magnetic moment respectively. Finally, the direct measurement of the magnetic order parameter for the C-AFM structure provided a value of the critical exponent β = 0.245 ≈ 1 4 , suggesting a non conventional critical behavior for the magnetic phase transition in NaCr₂O₄.