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The mixed-valent iridate Ba3InIr2O9 has been discussed as a promising candidate for quantum spin-liquid behavior. The compound exhibits Ir$^{4.5+}$ ions in face-sharing IrO6 octahedra forming Ir2O9 dimers with three t2g holes per dimer. Our results establish Ba3InIr2O9 as a cluster Mott insulator. Strong intra-dimer hopping delocalizes the three t2g holes in quasi-molecular dimer states while inter-dimer charge fluctuations are suppressed by Coulomb repulsion. The magnetism of Ba3InIr2O9 emerges from spin-orbit entangled quasi-molecular moments with yet unexplored interactions, opening up a new route to unconventional magnetic properties of 5d compounds. Using single-crystal x-ray diffraction we find the monoclinic space group C2/c already at room temperature. Dielectric spectroscopy shows insulating behavior. Resonant inelastic x-ray scattering (RIXS) reveals a rich excitation spectrum below 1.5 eV with a sinusoidal dynamical structure factor that unambiguously demonstrates the quasi-molecular character of the electronic states. Below 0.3 eV, we observe a series of excitations. According to exact diagonalization calculations, such low-energy excitations reflect the proximity of Ba3InIr2O9 to a hopping-induced phase transition based on the condensation of a quasi-molecular spin-orbit exciton. The dimer ground state roughly hosts two holes in a bonding j=1/2 orbital and the third hole in a bonding j=3/2 orbital., Comment: 14 pages, 10 figures, V2: published version, minor changes

$^7$Li nuclear magnetic resonance (NMR) and terahertz (THz) spectroscopies are used to probe magnetic excitations and their field dependence in the hyperhoneycomb Kitaev magnet $\beta$-Li$_2$IrO$_3$. Spin-lattice relaxation rate ($1/T_1$) measured down to 100\,mK indicates gapless nature of the excitations at low fields (below $H_c\simeq 2.8$\,T), in contrast to the gapped magnon excitations found in the honeycomb Kitaev magnet $\alpha$-RuCl$_3$ at zero applied magnetic field. At higher temperatures in $\beta$-Li$_2$IrO$_3$, $1/T_1$ passes through a broad maximum without any clear anomaly at the N\'eel temperature $T_N\simeq 38$\,K, suggesting the abundance of low-energy excitations that are indeed observed as two peaks in the THz spectra, both correspond to zone-center magnon excitations. At higher fields (above $H_c$), an excitation gap opens, and a re-distribution of the THz spectral weight is observed without any indication of an excitation continuum, in contrast to $\alpha$-RuCl$_3$ where an excitation continuum was reported., Comment: 6 pages, 4 figures

Detailed magnetization, specific heat, and $^7$Li nuclear magnetic resonance (NMR) measurements on single crystals of the hyperhoneycomb Kitaev magnet $\beta$-Li$_2$IrO$_3$ are reported. At high temperatures, {\cred anisotropy of the magnetization is reflected by the different Curie-Weiss temperatures for different field directions}, in agreement with the combination of a ferromagnetic Kitaev interaction ($K$) and a negative off-diagonal anisotropy ($\Gamma$) as two leading terms in the spin Hamiltonian. At low temperatures, magnetic fields applied along $a$ or $c$ have only a weak effect on the system and reduce the N\'eel temperature from 38 K at 0 T to about 35.5 K at 14 T, with no field-induced transitions observed up to 58 T on a powder sample. In contrast, the field applied along $b$ causes a drastic reduction in the $T_N$ that vanishes around $H_c=2.8$ T giving way to a crossover toward a quantum paramagnetic state. $^7$Li NMR measurements in this field-induced state reveal a gradual line broadening and a continuous evolution of the line shift with temperature, suggesting the development of local magnetic fields. The spin-lattice relaxation rate shows a peak around the crossover temperature 40 K and follows power-law behavior below this temperature., Comment: 10 pages, 9 figures; published version

We report the structural and magnetic properties of a new system LiRhMnO$_{4}$ (LRMO) through x-ray diffraction, bulk magnetization, heat capacity and $^{7}$Li nuclear magnetic resonance (NMR) measurements. LRMO crystallizes in the cubic space group $\mathit{Fd}$$\bar{3}$$\mathit{m}$. From the DC susceptibility data, we obtained the Curie-Weiss temperature $\mathrm{\theta}_{\mathrm{CW}}$ = -26 K and Curie constant $\mathit{C}$ = 1.79 Kcm$^{3}$/mol suggesting antiferromagnetic correlations among the magnetic Mn$^{4+}$ ions with an effective spin $\mathit{S}$ = $\frac{3}{2}$. At $\mathit{H}$ = 50 Oe, the field cooled and zero-field cooled magnetizations bifurcate at a freezing temperature, $T_{f}$ = 4.45 K, which yields the frustration parameter $\mathit{f=\frac{\mid\theta_{CW}\mid}{T_{f}}}>$5. AC susceptibility, shows a cusp-like peak at around $T_{f}$, with the peak position shifting as a function of the driving frequency, confirming a spin-glass-like transition in LRMO. LRMO also shows typical spin-glass characteristics such as memory effect, aging effect and relaxation. In the heat capacity, there is no sharp anomaly down to 2 K indicative of long-range ordering. The field sweep $^{7}$Li NMR spectra show broadening with decreasing temperature without any spectral line shift. The $^{7}$Li NMR spin-lattice and spin-spin relaxation rates also show anomalies due to spin freezing near $T_{f}$., Comment: 9 pages, 16 figures, 2 tables

We have investigated the structural and magnetic properties of a new cubic spinel LiZn$_{2}$V$_{3}$O$_{8}$ (LZVO) through x-ray diffraction, dc and ac susceptibility, magnetic relaxation, aging, memory effect, heat capacity and $^{7}$Li nuclear magnetic resonance (NMR) measurements. A Curie-Weiss fit of the dc susceptibility $\chi_{\mathrm{dc}}$($\mathit{T}$) yields a Curie-Weiss temperature $\mathrm{\theta}_{\mathrm{CW}}$ = -185 K. This suggests strong antiferromagnetic (AFM) interactions among the magnetic vanadium ions. The dc and ac susceptibility data indicate the spin-glass behavior below a freezing temperature $T_{f}$ $\simeq$ 3 K. The frequency dependence of the $T_{f}$ is characterized by the Vogel-Fulcher law and critical dynamic scaling behavior or power law. From both fitting, we obtained the value of the characteristic angular frequency $\omega_{0}$ $\approx$ 3.56$\times$10$^{6}$ Hz, the dynamic exponent $\mathit{zv}$ $\approx$ 2.65, and the critical time constant $\tau_{0}$ $\approx$ 1.82$\times$10$^{-6}$ s, which falls in the conventional range for typical cluster spin-glass (CSG) systems. The value of relative shift in freezing temperature $\delta T_{f}$ $\simeq$ 0.039 supports a CSG ground states. We also found aging phenomena and memory effects in LZVO. The asymmetric response of the magnetic relaxation below $T_{f}$ supports the hierarchical model. Heat capacity data show no long-range or short-range ordering down to 2 K. Only about 25% magnetic entropy change $(\Delta S_{\mathrm{m}})$ signifies the presence of strong frustration in the system. The $^{7}$Li NMR spectra show a shift and broadening with decreasing temperature. The spin-lattice and spin-spin relaxation rates show anomalies due to spin freezing around 3 K as the bulk magnetization., Comment: 12 pages, 17 figures, 2 tables

We report electron spin resonance (ESR) spectroscopy results on the double perovskite Ba$_2$YIrO$_6$. On general grounds, this material is expected to be nonmagnetic due to the strong coupling of the spin and orbital momenta of Ir$^{5+}$ (5$d^4$) ions. However, controversial experimental reports on either strong antiferromagnetism with static order at low temperatures or just a weakly paramagnetic behavior have triggered a discussion on the breakdown of the generally accepted scenario of the strongly spin-orbit coupled ground states in the 5$d^4$ iridates and the emergence of a novel exotic magnetic state. Our data evidence that the magnetism of the studied material is solely due to a few percent of Ir$^{4+}$ and Ir$^{6+}$ magnetic defects while the regular Ir$^{5+}$ sites remain nonmagnetic. Remarkably, the defect Ir$^{6+}$ species manifest magnetic correlations in the ESR spectra at $T\lesssim 20$ K suggesting a long-range character of superexchange in the double prevoskites as proposed by recent theories.

Temperature-pressure phase diagram of the Kitaev hyperhoneycomb iridate $\beta$-Li$_2$IrO$_3$ is explored using magnetization, thermal expansion, magnetostriction, and muon spin rotation ($\mu$SR) measurements, as well as single-crystal x-ray diffraction under pressure and ab initio calculations. The Neel temperature of $\beta$-Li$_2$IrO$_3$ increases with the slope of 0.9 K/GPa upon initial compression, but the reduction in the polarization field $H_c$ reflects a growing instability of the incommensurate order. At 1.4 GPa, the ordered state breaks down upon a first-order transition giving way to a new ground state marked by the coexistence of dynamically correlated and frozen spins. This partial freezing in the absence of any conspicuous structural defects may indicate classical nature of the resulting pressure-induced spin liquid, an observation paralleled to the increase in the nearest-neighbor off-diagonal exchange $\Gamma$ under pressure., Comment: 4 pages + Supplemental Material (published version)

The cubic double perovskite Ba$_2$YIrO$_6$ has been investigated by the local probe techniques nuclear magnetic resonance ($^{89}$Y NMR) and muon spin rotation (muSR). Both methods confirm the absence of magnetic long-range order in this compound but find evidence for diluted localized paramagnetic moments. NMR spin-lattice relaxation rate 1/T1 measurements suggest a slowing down of localized spin moments at low temperatures. An increase of the muSR spin-lattice relaxation rate lambda confirms the presence of weak magnetism in Ba$_2$YIrO$_6$ . However, these findings cannot be explained by the recently suggested excitonic type of magnetism. Instead, they point towards tiny amounts of localized paramagnetic spin centers leading to this magnetic response on the background of a simple nonmagnetic ground state of the 5d$^4$ ($J=0)$ electronic configuration of Ir$^{5+}$., Comment: 8 pages, 7 figures

Ba2YIrO6, a Mott insulator, with four valence electrons in Ir5+ d-shell (5d4) is supposed to be non-magnetic, with Jeff = 0, within the atomic physics picture. However, recent suggestions of non-zero magnetism have raised some fundamental questions about its origin. Focussing on the phonon dynamics, probed via Raman scattering, as a function of temperature and different incident photon energies, as an external perturbation. Our studies reveal strong renormalization of the phonon self-energy parameters and integrated intensity for first-order modes, especially redshift of the few first-order modes with decreasing temperature and anomalous softening of modes associated with IrO6 octahedra, as well as high energy Raman bands attributed to the strong anharmonic phonons and coupling with orbital excitations. The distinct renormalization of second-order Raman bands with respect to their first-order counterpart suggest that higher energy Raman bands have significant contribution from orbital excitations. Our observation indicates that strong anharmonic phonons coupled with electronic/orbital degrees of freedom provides a knob for tuning the conventional electronic levels for 5d-orbitals, and this may give rise to non-zero magnetism as postulated in recent theoretical calculations with rich magnetic phases.

Materials with a 5d4 electronic configuration are generally considered to have a nonmagnetic ground state (J=0). Interestingly, Sr2YIrO6 (Ir5+ having 5d4 electronic configuration) was recently reported to exhibit long-range magnetic order at low temperature and the distorted IrO6 octahedra were discussed to cause the magnetism in this material. Hence, a comparison of structurally distorted Sr2YIrO6 with cubic Ba2YIrO6 may shed light on the source of magnetism in such Ir5+ materials with 5d4 configuration. Besides, Ir5+ materials having 5d4 are also interesting in the context of recently predicted excitonic types of magnetism. Here we report a single-crystal-based analysis of the structural, magnetic, and thermodynamic properties of Ba2YIrO6. We observe that in Ba2YIrO6 for temperatures down to 0.4 K, long-range magnetic order is absent but at the same time correlated magnetic moments are present. We show that these moments are absent in fully relativistic ab initio band-structure calculations; hence, their origin is presently unclear., Comment: 8 pages, 9 figures

CoAl2O4 spinel with magnetic Co2+ ions on the diamond A-lattice is known to be magnetically frustrated. We compare neutron single crystal diffraction patterns measured in zero and applied magnetic fields with the ones obtained from classical Monte-Carlo models. In simulations we test the influence of various parameters on diffraction patterns: the ratio of nearest-, J1, and next-nearest, J2, neighbor interactions, magnetic field applied along the principal crystallographic directions, and random disorder on the A(Co2+)- and B(Al3+)- sites. We conclude that the models considered so far explain the broadening of magnetic Bragg peaks in zero magnetic field and their anisotropic response to applied magnetic field only partly. As bulk properties of our single crystal are isotropic, we suggest that its microstructure, specifically <111>-twin boundaries, could be a reason of the nonconventional magnetic order in CoAl2O4., Comment: 9 pages, 8 figures