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Register a new userThe Curious Case of NiRh$_2$O$_4$: A Spin-Orbit Entangled Diamond Lattice Paramagnet
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Motivated by the interest in topological quantum paramagnets in candidate spin-$1$ magnets, we investigate the diamond lattice compound NiRh$_2$O$_4$ using {it ab initio} theory and model Hamiltonian approaches. Our density functional study, taking into account the unquenched orbital degrees of freedom, shows stabilization of $S=1$ and $L=1$ state. We highlight the importance of spin-orbit coupling, in addition to Coulomb correlations, in driving the insulating gap, and uncover frustrating large second-neighbor exchange mediated by Ni-Rh covalency. A single-site model Hamiltonian incorporating the large tetragonal distortion is shown to give rise to a spin-orbit entangled non-magnetic ground state, largely accounting for the entropy, magnetic susceptibility, and inelastic neutron scattering results. Incorporating inter-site exchange within a slave-boson theory, we show that exchange frustration can suppress exciton condensation. We capture the dispersive gapped magnetic modes, uncover `dark states invisible to neutrons, and make predictions for future experiments.
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We determined the magnetic structure of CuCr$_2$O$_4$ using neutron diffraction and irreducible representation analysis. The measurements identified a new phase between 155 K and 125 K as nearly collinear magnetic ordering in the Cr pyrochlore lattice. Below 125 K, a Cu-Cr ferrimagnetic component develops the noncollinear order. Along with the simultaneously obtained O positions and the quantum effect of spin-orbit coupling, the magnetic structure is understood to involve spin-orbit ordering, accompanied by an appreciably deformed orbital of presumably spin-only Cu and Cr.
Spin fluctuations were studied over a wide momentum ($hbar Q$) and energy ($E$) space in the frustrated $d$-electron heavy-fermion metal LiV$_2$O$_4$ by time-of-flight inelastic neutron scattering. We observed the overall $Q$$-$$E$ evolutions near the characteristic $Q=0.6$ {AA}$^{-1}$ peak and found another weak broad magnetic peak around 2.4 {AA}$^{-1}$. The data are described by a simple response function, a highly itinerant magnetic form factor, and antiferromagnetic short-range spatial correlations, indicating that heavy-fermion formation is attributable to spin-orbit fluctuations with orbital hybridization.
We describe powder and single-crystal inelastic neutron scattering experiments on a spinel-type antiferromagnet GeCo$_2$O$_4$, represented by an effective total angular momentum J_eff = 1/2. Several types of non-dispersive short-range magnetic excitations were discovered. The scattering intensity maps in $vec{Q}$ space are well reproduced by dynamical structure factor analyses using molecular model Hamiltonians. The results of analyses strongly suggest that the molecular excitations below T_N arise from a hidden molecular-singlet ground state, in which ferromagnetic subunits are antiferromagnetically coupled. The quasielastic excitations above T_N are interpreted as its precursor. A combination of frustration and J_eff = 1/2 might induce these quantum phenomena.
We report single-crystal neutron diffraction studies on a spinel antiferromagnet GeCo$_2$O$_4$, which exhibits magnetic order with a trigonal propagation vector and tetragonal lattice expansion ($c/asimeq1.001$) below $T_{rm N}=21$ K. For this inconsistency between spin and lattice in symmetry, magnetic Bragg reflections with a tetragonal propagation vector were discovered below $T_{rm N}$. We discuss spin and orbital states of Co$^{2+}$ ion underlying the new magnetic component.
Calcium vanadate CaV$_2$O$_4$ has a crystal structure of quasi-one-dimensional zigzag chains composed of orbital-active V$^{3+}$ ions and undergoes successive structural and antiferromagnetic phase transitions at $T_ssim 140$ K and $T_N sim 70$ K, respectively. We perform ultrasound velocity measurements on a single crystal of CaV$_2$O$_4$. The temperature dependence of its shear elastic moduli exhibits huge Curie-type softening upon cooling that emerges above and below $T_s$ depending on the elastic mode. The softening above $T_s$ suggests the presence of either onsite Jahn-Teller-type or intersite ferro-type orbital fluctuations in the two inequivalent V$^{3+}$ zigzag chains. The softening below $T_s$ suggests the occurrence of a dimensional spin-state crossover, from quasi-one to three, that is driven by the spin-lattice coupling along the inter-zigzag-chain orthogonal direction. The successive emergence of the orbital- and spin-driven lattice instabilities above and below $T_s$, respectively, is unique to the orbital-spin zigzag chain system of CaV$_2$O$_4$.
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