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Bulk studies have revealed a first-order valence phase transition in Ba$_2$PrRu$_{1-x}$Ir$_x$O$_6$ ($0.10 \le x \le 0.25$), which is absent in the parent compounds with $x = 0$ (Pr$^{3+}$) and $x =1$ (Pr$^{4+}$), which exhibit antiferromagnetic order with transition temperatures $T_{\rm N} = 120$ and 72 K, respectively. In the present study, we have used magnetization, heat capacity, neutron diffraction, inelastic neutron scattering and x-ray absorption measurements to investigate the nature of the Pr ion in $x =0.1$. The magnetic susceptibility and heat capacity of $x =0.1$ show a clear sign of the first order valence phase transition below 175 K, where the Pr valence changes from 3+ to 4+. Neutron diffraction analysis reveals that $x =0.1$ crystallizes in a monoclinic structure with space group $P2_1/n$ at 300 K, but below 175 K two phases coexist, the monoclinic having the Pr ion in a 3+ valence state and a cubic one ($Fm\overline{3}m$) having the Pr ion in a 4+ valence state. Clear evidence of an antiferromagnetic ordering of the Pr and Ru moments is found in the monoclinic phase of the $x = 0.1$ compound below 110 K in the neutron diffraction measurements. Meanwhile the cubic phase remains paramagnetic down to 2 K, a temperature below which heat capacity and susceptibility measurements reveal a ferromagnetic ordering. High energy inelastic neutron scattering data reveal well-defined high-energy magnetic excitations near 264 meV at temperatures below the valence transition. The high energy excitations are assigned to the Pr$^{4+}$ ions in the cubic phase and the low energy excitations to the Pr$^{3+}$ ions in the monoclinic phase. Further direct evidence of the Pr valence transition has been obtained from the x-ray absorption spectroscopy., Comment: 10 pages and 10 figures

Sr$_{3}$ZnIrO$_{6}$ is an effective spin one-half Mott insulating iridate belonging to a family of magnets which includes a number of quasi-one dimensional systems as well as materials exhibiting three dimensional order. Here we present the results of an extensive investigation into the magnetism including heat capacity, a.c. susceptibility, muon spin rotation ($\mu$SR), neutron diffraction and inelastic neutron scattering on the same sample. It is established that the material exhibits a transition at about $17$ K into a three-dimensional antiferromagnetic structure with propagation vector $\boldsymbol{k}=(0,\frac{1}{2},1)$ in the hexagonal setting of R$\bar{3}$c and non-collinear moments of $0.87$$\mu_B$ on Ir$^{4+}$ ions. Further we have observed a well defined powder averaged spin wave spectrum with zone boundary energy of $\sim 5$ meV at $5$ K. We stress that a theoretical analysis shows that the observed non-collinear magnetic structure arises from anisotropic inter- and intra- chain exchange which has its origin in significant spin-orbit coupling. The model can satisfactorily explain the observed spin wave excitations., Comment: 6 pages, 5 figures

Inelastic neutron scattering experiments have been carried out to determine the crystal field states of the Kondo lattice heavy fermions CeRuSn3 and CeRhSn3. Both the compounds crystallize in LaRuSn3-type cubic structure (space group Pm-3n) in which the Ce atoms occupy two distinct crystallographic sites with cubic (m-3) and tetragonal (-4m.2) point symmetries. The INS data of CeRuSn3 reveal the presence of a broad excitation centered around 6-8 meV which is accounted by a model based on crystal electric field (CEF) excitations. On the other hand, the INS data of isostructural CeRhSn3 reveal three CEF excitations around 7.0, 12.2 and 37.2 meV. The neutron intensity sum rule indicates that the Ce ions at both cubic and tetragonal Ce sites are in Ce3+ state in both CeRuSn3 and CeRhSn3. The CEF level schemes for both the compounds are deduced. We estimate the Kondo temperature T_K = 3.1(2) K for CeRuSn3 from neutron quasielastic linewidth in excellent agreement with that determined from the scaling of magnetoresistance which gives T_K = 3.2(1) K. For CeRhSn3 the neutron quasielastic linewidth gives T_K = 4.6 K. For both CeRuSn3 and CeRhSn3, the ground state of Ce3+ turns out to be a quartet for the cubic site and a doublet for the tetragonal site., Comment: 12 pages, 13 figures, 2 tables, to appear in Phys. Rev. B

The newly discovered Ising-type ferromagnet CeRu$_2$Al$_2$B exhibits an additional phase transition at $T_\textrm{N}$ = 14.2 K before entering the ferromagnetic ground state at $T_\textrm{C}$ = 12.8 K. We clarify the nature of this transition through high resolution neutron diffraction measurements. The data reveal the presence of a longitudinal incommensurate spin-density wave (SDW) in the temperature range of $T_\textrm{C}

We have investigated the non-centrosymmetric tetragonal heavy-fermion compound CeAuAl3 using muon spin rotation (muSR), neutron diffraction (ND) and inelastic neutron scattering (INS) measurements. We have also revisited the magnetic, transport and thermal properties. The magnetic susceptibility reveals an antiferromagnetic transition at 1.1 K with a possibility of another magnetic transition near 0.18 K. The heat capacity shows a sharp lambda-type anomaly at 1.1 K in zero-filed, which broadens and moves to higher temperature in applied magnetic field. Our zero-field muSR and ND measurements confirm the existence of a long-range magnetic ground state below 1.2 K. Further the ND study reveals an incommensurate magnetic ordering with a magnetic propagation vector k = (0, 0, 0.52) and a spiral structure of Ce moments coupled ferromagnetically within the ab-plane. Our INS study reveals the presence of two well-defined crystal electric field (CEF) excitations at 5.1 meV and 24.6 meV in the paramagnetic phase of CeAuAl3 which can be explained on the basis of the CEF theory. Furthermore, low energy quasi-elastic excitations show a Gaussian line shape below 30 K compared to a Lorentzian line shape above 30 K, indicating a slowdown of spin fluctuation below 30 K. We have estimated a Kondo temperature of TK=3.5 K from the quasi-elastic linewidth, which is in good agreement with that estimated from the heat capacity. This study also indicates the absence of any CEF-phonon coupling unlike that observed in isostructural CeCuAl3. The CEF parameters, energy level scheme and their wave functions obtained from the analysis of INS data explain satisfactorily the single crystal susceptibility in the presence of two-ion anisotropic exchange interaction in CeAuAl3., Comment: 28 pages and 17 figures

The results of heat capacity C_p(T, H) and electrical resistivity \rho(T,H) measurements down to 0.35 K as well as muon spin relaxation and rotation (\muSR) measurements on a noncentrosymmetric superconductor LaIrSi3 are presented. Powder neutron diffraction confirmed the reported noncentrosymmetric body-centered tetragonal BaNiSn3-type structure (space group I4\,mm) of LaIrSi3. The bulk superconductivity is observed below T_c = 0.72(1) K. The intrinsic \Delta C_e/\gamma_n T_c = 1.09(3) is significantly smaller than the BCS value of 1.43, and this reduction is accounted by the \alpha-model of BCS superconductivity. The analysis of the superconducting state C_e(T) data by the single-band \alpha-model indicates a moderately anisotropic order parameter with the s-wave gap \Delta(0)/k_B T_c = 1.54(2) which is lower than the BCS value of 1.764. Our estimates of various normal and superconducting state parameters indicate a weakly coupled electron-phonon driven type-I s-wave superconductivity in LaIrSi3. The \muSR results also confirm the conventional type-I superconductivity in LaIrSi3 with a preserved time reversal symmetry and hence a singlet pairing superconducting ground state., Comment: 11 pages, 8 figures, 2 tables

The magnetic state of the noncentrosymmetric antiferromagnet CeNiC$_2$ has been studied by magnetic susceptibility, heat capacity, muon spin relaxation ($\mu$SR) and inelastic neutron scattering (INS) measurements. CeNiC$_2$ exhibits three magnetic phase transitions at $T_{N_1}$ = 20 K, $T_{N_2}$ = 10 K and $T_{N_3}$ = 2.5 K. The presence of long range magnetic order below 20 K is confirmed by the observation of oscillations in the $\mu$SR spectra between 10 and 20 K and a sharp increase in the muon depolarization rate. INS studies reveal two well-defined crystal electric field (CEF) excitations around 8 and 30 meV. INS data have been analyzed using a CEF model and the wave functions were evaluated. We also calculated the direction and magnitude of the ground state moment using CEF wave functions and compare the results with that proposed from the neutron diffraction. Our CEF model correctly predicts that the moments order along the $b-$axis (or $y$-axis) and the observed magnetic moment is 0.687(5) $\mu_B$, which is higher than the moment observed from the neutron diffraction (0.25 $\mu_B$/Ce). We attribute the observed reduced moment due to the Kondo screening effect., Comment: 10 pages, 13 figures

We use neutron diffraction, magnetometry and low temperature heat capacity to probe giant magneto-elastic coupling in CoMnSi-based antiferromagnets and to establish the origin of the entropy change that occurs at the metamagnetic transition in such compounds. We find a large difference between the electronic density of states of the antiferromagnetic and high magnetisation states. The magnetic field-induced entropy change is composed of this contribution and a significant counteracting lattice component, deduced from the presence of negative magnetostriction. In calculating the electronic entropy change, we note the importance of using an accurate model of the electronic density of states, which here varies rapidly close to the Fermi energy., Comment: 11 pages, 9 figures. Figures 4 and 6 were updated in v2 of this preprint. In v3, figures 1 and 2 have been updated, while Table II and the abstract have been extended. In v4, Table I has updated with relevant neutron diffraction data

We have carried out neutron diffraction, muon spin relaxation (muSR) and inelastic neutron scattering investigations on a polycrystalline sample of CeOs2Al10 to investigate the nature of the phase transition observed near 29 K in the resistivity and heat capacity. Our muSR data clearly reveal coherent frequency oscillations below 28 K, indicating the presence of an internal field at the muon site, which confirms the long-range magnetic ordering of the Ce-moment below 28 K. Upon cooling the sample below 15 K, unusual behaviour of the temperature dependent muSR frequencies may indicate either a change of the muon site, consistent with the observation of superstructure reflections in electron diffraction or a change of the ordered magnetic structure. Neutron diffraction data do not reveal any clear sign of either magnetic Bragg peaks or superlattice reflections. Furthermore, inelastic neutron scattering (INS) measurements clearly reveal the presence of a sharp inelastic excitation near 11 meV between 5 K and 26 K, due to opening of a gap in the spin excitation spectrum, which transforms into a broad response at and above 30 K. The magnitude of the spin-gap (11 meV) as derived from the INS peak position agrees very well with the gap value as estimated from the bulk properties., Comment: 37 pages

We have carried out neutron powder-diffraction measurements on zinc paratacamite Zn$_x$Cu$_{4-x}$(OH)$_6$Cl$_2$ with $x=1$, and studied the heat capacity in fields of up to 9 T for $0.5 \leq x \leq 1$. The $x=1$ phase has recently been shown to be an outstanding realisation of the $S=1/2$ kagom\'{e} antiferromagnet. A weak mixing of Cu$^{2+}$/Zn$^{2+}$ between the Cu and the Zn sites, corresponding to $\sim 9$% of all Cu$^{2+}$ for $x=1$, is observed using neutron diffraction. This ``antisite disorder'' provides a consistent explanation of the field dependence of the heat capacity for $0.8 \leq x \leq 1$. From comparison of the derived Cu$^{2+}$ occupancy of the Zn sites for $x = 0.8... 1$ with the magnetic susceptibility, we argue that for $x = 0.8... 1$ zinc paratacamite is a spin liquid without a spin gap. The presence of unpaired but nevertheless strongly interacting spins gives rise to a macroscopically degenerate ground state manifold, with increasingly glassy dynamics as $x$ is lowered., Comment: Thorough revision of manuscript. Added 1 figure. Manuscript submitted to Physics Review Letters

The magnetic ground state of the antiferromagnet Kondo lattice compound Ce8Pd24Ga has been investigated using neutron powder diffraction, inelastic neutron scattering and zero-field muon spin relaxation measurements. The neutron diffraction analysis, below TN (3.6(0.2)K), reveals a commensurate type-C antiferromagnetic structure with the ordered state magnetic moment of \~0.36 mB/Ce-atom along the cubic <111> direction. The analysis of the inelastic neutron scattering (INS) data based on the crystal field (CF) model reveals a doublet ground state with a ground state moment of 1.29 mB/Ce-atom. The observed magnetic moment from neutron diffraction, which is small compared to the expected value from CF-analysis, is attributed to screening of the local Ce moment by the Kondo effect. This is supported by the observed Kondo-type resistivity and a small change in the entropy of Ce8Pd24Ga at TN. The zero-field muon spin relaxation rate exhibits a sharp increase below TN indicating ordering of Ce moments, in agreement with the neutron diffraction data. The present studies reveal that the physical properties of Ce8Pd24Ga are governed by the onsite Kondo compensation, the moment stabilizing intersite RKKY interaction and the crystal field effect., Comment: 11 pages and 7Figs, Phys. Rev. B (accepted)