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Spin-orbital correlations from complex orbital order in MgV$_{2}$O$_{4}$

Strongly Correlated Electrons 2023-11-15 v1 Materials Science

Abstract

MgV2_{2}O4_{4} is a spinel based on magnetic V3+^{3+} ions which host both spin (S=1S=1) and orbital (leff=1l_{eff}=1) moments. Owing to the underlying pyrochlore coordination of the magnetic sites, the spins in MgV2_{2}O4_{4} only antiferromagnetically order once the frustrating interactions imposed by the Fd3mFd\overline{3}m lattice are broken through an orbitally-driven structural distortion at TS_{S} \simeq 60 K. Consequently, a N\'eel transition occurs at TN_{N} \simeq 40 K. Low temperature spatial ordering of the electronic orbitals is fundamental to both the structural and magnetic properties, however considerable discussion on whether it can be described by complex or real orbital ordering is ambiguous. We apply neutron spectroscopy to resolve the nature of the orbital ground state and characterize hysteretic spin-orbital correlations using x-ray and neutron diffraction. Neutron spectroscopy finds multiple excitation bands and we parameterize these in terms of a multi-level (or excitonic) theory based on the orbitally degenerate ground state. Meaningful for the orbital ground state, we report an "optical-like" mode at high energies that we attribute to a crystal-field-like excitation from the spin-orbital jeffj_{eff}=2 ground state manifold to an excited jeffj_{eff}=1 energy level. We parameterize the magnetic excitations in terms of a Hamiltonian with spin-orbit coupling and local crystalline electric field distortions resulting from deviations from perfect octahedra surrounding the V3+^{3+} ions. We suggest that this provides compelling evidence for complex orbital order in MgV2_{2}O4_{4}. We then apply the consequences of this model to understand hysteretic effects in the magnetic diffuse scattering where we propose that MgV2_{2}O4_{4} displays a high temperature orbital memory of the low temperature spin order.

Keywords

Cite

@article{arxiv.2309.06853,
  title  = {Spin-orbital correlations from complex orbital order in MgV$_{2}$O$_{4}$},
  author = {H. Lane and P. M. Sarte and K. Guratinder and A. M. Arevalo-Lopez and R. S. Perry and E. C. Hunter and T. Weber and B. Roessli and A. Stunault and Y. Su and R. A. Ewings and S. D. Wilson and P. Böni and J. P. Attfield and C. Stock},
  journal= {arXiv preprint arXiv:2309.06853},
  year   = {2023}
}

Comments

21 pages and 13 figures

R2 v1 2026-06-28T12:20:10.946Z