We studied the Co valences and spin states in electron-doped LaCo$_{1-y}$Te$_{y}$O$_3$ by measuring x-ray absorption spectra and electron spin resonance. The low-temperature insulating state involves the low-spin Co$^{3+}$ ($S=0$) and the high-spin C
o$^{2+}$ state, which is described by $g=3.8$ and $j_{rm eff}=1/2$. The results, in concurrence with the electron-hole asymmetry confirmed in electrical resistivity, coincide with a spin-blockade phenomenon in this system. Further, we discuss the $g$ factor in terms of the strong covalent-bonding nature and consider multiple origins of this phenomenon.
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 th
e 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 studied the spin-state responses to light impurity doping in low-spin perovskite LaCoO$_{3}$ (Co^3+: d^6) through magnetization and X-ray fluorescence measurements of single-crystal LaCo$_{0.99}$$M_{0.01}$O$_{3}$ ($M$ = Cr, Mn, Fe, Ni). In the mag
netization curves measured at 1.8 K, a change in the spin-state was not observed for Cr, Mn, or Fe doping but was observed for Ni doping. Strong magnetic anisotropy along the [100] easy axis was also found in the Ni-doped sample. The fluorescence measurements revealed that the valences were roughly estimated to be Cr^3+, Mn^4+, Fe^(3+delta)+, and Ni^3+. From the observed chemical trends, we propose that the chemical potential is a key factor in inducing the change of the low-spin state. By expanding a model of the ferromagnetic spin-state heptamer generated by hole doping, we discuss the emergence of highly anisotropic ferromagnetic spin-state clusters induced by low-spin Ni^3+ with Jahn-Teller activity. We also discuss applicability of the present results to mantle materials and impurity-doped pyrites with Fe (d^6).
High degeneracy in ground states leads to the generation of exotic zero-energy modes, a representative example of which is the formation of molecular spin liquid-like fluctuations in a frustrated magnet. Here we present single-crystal inelastic neutr
on scattering results for the frustrated magnet MgCr$_2$O$_4$, which show that a common set of finite-energy molecular spin excitation modes is sustained in both the liquid-like paramagnetic phase and a magnetically ordered phase with an extremely complex structure. Based on this finding, we propose the concept of high degeneracy in excited states, which promotes local resonant elementary excitations. This concept is expected to have ramifications on our understanding of excitations in many complex systems, including not only spin but also atomic liquids, complex order systems, and amorphous systems.
The spin-frustrated conductor Mn$_3$Pt exhibits a characteristic magnetic structure called partial disorder in which some spin sites can form magnetic order through the generation of non-ordered sites that locally relieve the frustration. Here we rep
ort the results of a single-crystal inelastic neutron scattering study of this compound. The measured momentum $vec{Q}$ correlations of diffusive magnetic scattering reveal that the paramagnetic phase exhibits short-range spin fluctuations with the same type of partial disorder. Its relation to conductivity is also discussed.
We describe a method of white-beam inelastic neutron scattering for improved measurement efficiency. The method consists of matrix inversion and selective extraction. The former is to resolve each incident energy component from the white-beam data, a
nd the latter eliminates contamination by elastic components, which produce strong backgrounds that otherwise obfuscate the inelastic scattering components. In this method, the optimal experimental condition to obtain high efficiency will strongly depend on the specific aim of the individual experiments.
In this study, we performed powder neutron diffraction and inelastic scattering measurements of frustrated pyrochlore Nd$_2$Ir$_2$O$_7$, which exhibits a metal-insulator transition at a temperature $T_{rm MI}$ of 33 K. The diffraction measurements re
vealed that the pyrochlore has an antiferromagnetic long-range structure with propagation vector $vec{q}_{0}$ of (0,0,0) and that it grows with decreasing temperature below 15 K. This structure was analyzed to be of the all-in all-out type, consisting of highly anisotropic Nd$^{3+}$ magnetic moments of magnitude $2.3pm0.4$$mu_{rm B}$, where $mu_{rm B}$ is the Bohr magneton. The inelastic scattering measurements revealed that the Kramers ground doublet of Nd$^{3+}$ splits below $T_{rm MI}$. This suggests the appearance of a static internal magnetic field at the Nd sites, which probably originates from a magnetic order consisting of Ir$^{4+}$ magnetic moments. Here, we discuss a magnetic structure model for the Ir order and the relation of the order to the metal-insulator transition in terms of frustration.
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 excita
tions 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 incons
istency 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.
We measured two magnetic modes with finite and discrete energies in an antiferromagnetic ordered phase of a geometrically frustrated magnet MgCr2O4 by single-crystal inelastic neutron scattering, and clarified the spatial spin correlations of the two
levels: one is an antiferromagnetic hexamer and the other is an antiferromagnetic heptamer. Since these correlation types are emblematic of quasielastic scattering with geometric frustration, our results indicate instantaneous suppression of lattice distortion in an ordered phase by spin-lattice coupling, probably also supported by orbital and charge. The common features in the two levels, intermolecular independence and discreteness of energy, suggest that the spin molecules are interpreted as quasiparticles (elementary excitations with energy quantum) of highly frustrated spins, in analogy with the Fermi liquid approximation.
