The spinel vanadates have become a model family for exploring orbital order on the frustrated pyrochlore lattice, and recent debate has focused on the symmetry of local crystal fields at the cation sites. Here, we present neutron scattering measureme
nts of the magnetic excitation spectrum in $mathrm{FeV_2O_4}$, a recent example of a ferrimagnetic spinel vanadate which is available in single crystal form. We report the existence of two emergent magnon modes at low temperatures, which draw strong parallels with the closely related material, $mathrm{MnV_2O_4}$. We were able to reproduce the essential elements of both the magnetic ordering pattern and the dispersion of the inelastic modes with semi- classical spin wave calculations, using a minimal model that implies a sizeable single-ion anisotropy on the vanadium sublattice. Taking into account the direction of ordered spins, we associate this anisotropy with the large trigonal distortion of $mathrm{VO_6}$ octahedra, previously observed via neutron powder diffraction measurements. We further report on the spin gap, which is an order-of-magnitude larger than that observed in $mathrm{MnV_2O_4}$. By looking at the overall temperature dependence, we were able to show that the gap magnitude is largely associated with the ferro-orbital order known to exist on the iron sublattice, but the contribution to the gap from the vanadium sublattice is in fact comparable to what is reported in the Mn compound. This reinforces the conclusion that the spin canting transition is associated with the ordering of vanadium orbitals in this system, and closer analysis indicates closely related physics underlying orbital transitions in $mathrm{FeV_2O_4}$ and $mathrm{MnV_2O_4}$.
The usual classical behaviour of S = 3/2, B-site ordered double perovskites generally results in simple, commensurate magnetic ground states. In contrast, heat capacity and neutron powder diffraction measurements for the S = 3/2 systems La2NaBO6 (B =
Ru, Os) reveal an incommensurate magnetic ground state for La2NaRuO6 and a drastically suppressed ordered moment for La2NaOsO6. This behaviour is attributed to the large monoclinic structural distortions of these double perovskites. The distortions have the effect of weakening the nearest neighbour superexchange interactions, presumably to an energy scale that is comparable to the next nearest neighbour superexchange. The exotic ground states in these materials can then arise from a competition between these two types of antiferromagnetic interactions, providing a novel mechanism for achieving frustration in the double perovskite family.
The vibrational excitations of crystalline solids corresponding to acoustic or optic one phonon modes appear as sharp features in measurements such as neutron spectroscopy. In contrast, many-phonon excitations generally produce a complicated, weak, a
nd featureless response. Here we present time-of-flight neutron scattering measurements for the binary solid uranium nitride (UN), showing well-defined, equally-spaced, high energy vibrational modes in addition to the usual phonons. The spectrum is that of a single atom, isotropic quantum harmonic oscillator and characterizes independent motions of light nitrogen atoms, each found in an octahedral cage of heavy uranium atoms. This is an unexpected and beautiful experimental realization of one of the fundamental, exactly-solvable problems in quantum mechanics. There are also practical implications, as the oscillator modes must be accounted for in the design of generation IV nuclear reactors that plan to use UN as a fuel.
We present a neutron diffraction study of FeV2O4, which is rare in exhibiting spin and orbital degrees of freedom on both cation sublattices of the spinel structure. Our data confirm the existence of three structural phase transitions previously iden
tified with x-ray powder diffraction, and reveal that the lower two transitions are associated with sequential collinear and canted ferrimagnetic transitions involving both cation sites. Through consideration of local crystal and spin symmetry, we further conclude that Fe2+ cations are ferro-orbitally ordered below 135K and V3+ orbitals order at 60K in accordance with predictions for vanadium spinels with large trigonal distortions and strong spin-orbit coupling. Intriguingly, the direction of ordered vanadium spins at low temperatures obey `ice rules more commonly associated with the frustrated rare-earth pyrochlore systems.
Two B-site ordered double perovskites, La2LiMoO6 and Ba2YMoO6, based on the S = 1/2 ion, Mo5+, have been investigated in the context of geometric magnetic frustration. Powder neutron diffraction, heat capacity, susceptibility, muon spin relaxation(_S
R), and 89Y NMR- including MAS NMR- data have been collected. La2LiMoO6 deviates strongly from simple Curie-Weiss paramagnetic behavior below 150K and zero-field cooled/ field cooled (ZFC/FC)irreversibility occurs below 20K with a weak, broad susceptibility maximum near 5K in the ZFC data. A Curie-Weiss fit shows a reduced mu_eff=1.42mu_B, (spin only = 1.73 muB) and a Weiss temperature, theta_c, which depends strongly on the temperature range of the fit. Powder neutron diffraction, heat capacity and 7Li NMR show no evidence for long range magnetic order to 2K. On the other hand oscillations develop below 20K in muSR indicating at least short range magnetic correlations. Susceptibility data for Ba2YMoO6 also deviate strongly from the C-W law below 150K with a similarly reduced mu_eff = 1.72mu_B and theta_c = - 219(1)K. Heat capacity, neutron powder diffraction and muSR data show no evidence for long range order to 2K but a very broad maximum appears in the heat capacity. The 89Y NMR paramagnetic Knight shift shows a remarkable local spin susceptibility behavior below about 70K with two components from roughly equal sample volumes, one indicating a singlet state and the other a strongly fluctuating paramagnetic state. Further evidence for a singlet state comes from the behavior of the relaxation rate, 1/T1. These results are discussed and compared with those from other isostructural S = 1/2 materials and those based on S = 3/2 and S = 1.
We report muon spin relaxation ($mu$SR) and magnetic susceptibility measurements on Cu(Cl,Br)La(Nb,Ta)$_{2}$O$_{7}$, which demonstrate: (a) the absence of static magnetism in (CuCl)LaNb$_{2}$O$_{7}$ down to 15 mK confirming a spin-gapped ground state
; (b) phase separation between partial volumes with a spin-gap and static magnetism in (CuCl)La(Nb,Ta)$_{2}$O$_{7}$; (c) history-dependent magnetization in the (Nb,Ta) and (Cl,Br) substitution systems; (d) a uniform long-range collinear antiferromagnetic state in (CuBr)LaNb$_{2}$O$_{7}$; and (e) a decrease of Neel temperature with decreasing Br concentration $x$ in Cu(Cl$_{1-x}$Br$_{x}$)LaNb$_{2}$O$_{7}$ with no change in the ordered Cu moment size for $0.33 leq x leq 1$. Together with several other $mu$SR studies of quantum phase transitions in geometrically-frustrated spin systems, the present results reveal that the evolution from a spin-gap to a magnetically ordered state is often associated with phase separation and/or a first order phase transition.
The recent discovery and subsequent developments of FeAs-based superconductors have presented novel challenges and opportunities in the quest for superconducting mechanisms in correlated-electron systems. Central issues of ongoing studies include int
erplay between superconductivity and magnetism as well as the nature of the pairing symmetry reflected in the superconducting energy gap. In the cuprate and RE(O,F)FeAs (RE = rare earth) systems, the superconducting phase appears without being accompanied by static magnetic order, except for narrow phase-separated regions at the border of phase boundaries. By muon spin relaxation measurements on single crystal specimens, here we show that superconductivity in the AFe$_{2}$As$_{2}$ (A = Ca,Ba,Sr) systems, in both the cases of composition and pressure tunings, coexists with a strong static magnetic order in a partial volume fraction. The superfluid response from the remaining paramagnetic volume fraction of (Ba$_{0.5}$K$_{0.5}$)Fe$_{2}$As$_{2}$ exhibits a nearly linear variation in T at low temperatures, suggesting an anisotropic energy gap with line nodes and/or multi-gap effects.
Zero-field (ZF) muon spin relaxation ($mu$SR) measurements have revealed static commensurate magnetic order of Fe moments in NdOFeAs below $T_{N} sim 135$ K, with the ordered moment size nearly equal to that in LaOFeAs, and confirmed similar behavior
in BaFe$_{2}$As$_{2}$. In single crystals of superconducting (Ba$_{0.55}$K$_{0.45}$)Fe$_{2}$As$_{2}$, $mu$SR spectra indicate static magnetism with incommensurate or short-ranged spin structure in $sim$ 70 % of volume below $T_{N} sim$ 80 K, coexisting with remaining volume which exhibits superfluid-response consistent with nodeless gap below $T_{c}sim 30$ K.
We have performed zero-field muon spin rotation measurements on single crystals of La_{2-x}Sr_{x}CuO_{4} to search for spontaneous currents in the pseudo-gap state. By comparing measurements on materials across the phase diagram, we put strict upper
limits on any possible time-reversal symmetry breaking fields that could be associated with the pseudo-gap. Comparison between experimental limits and proposed circulating current states effectively eliminates the possibility that such states exist in this family of materials.
