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The pyrochlore osmate Ho2Os2O7 is a candidate material for a fragile J=0 local singlet ground state, however little is known regarding the single-ion behavior of either the Os or Ho ions. To address this we present polarized neutron powder diffraction (PNPD) and resonant inelastic x-ray scattering (RIXS) measurements that separately probe the local site behavior of the Os and Ho ions. The PNPD results are dominated by Ho3+ scattering and the analysis reveals local site susceptibility behavior consistent with spin ice materials. Complimentary unpolarized neutron powder diffraction show an ordered spin ice ground state in an applied magnetic field. To isolate the Os4+ single-ion behavior we present resonant inelastic x-ray scattering (RIXS) measurements at the osmium L-edge. Analysis of the RIXS spectra parameterize the spin-orbit coupling (0.35 eV), Hund's coupling (0.27 eV) and trigonal distortion (-0.17 eV). The results are considered within the context of a J=0 model and possible departures from this through structural distortions, excitonic interactions and 5d-4f interactions between the Os ion and the surrounding Ho lattice. The experimental methodology employed highlights the complimentary information available in rare earth based 5d pyrochlores from distinct neutron and x-ray scattering techniques that allow for the isolation and determination of the behavior of the different ions.

The magnetic properties of [Mn(pyrazinecarboxylate)2]n (Mn-pyrazine), empirical formula C10H6MnN4O4, are investigated through susceptibility, heat capacity and neutron scattering measurements. The structure of Mn-pyrazine consists of Mn-Mn dimers linked on a distorted 2D hexagonal structure. The weak out of plane interactions create a quasi-2D magnetic material within the larger three dimensional metal organic framework (MOF) structure. We show that this material undergoes a two stage magnetic transition, related to the low dimensionality of the Mn lattice. First at 5 K, which is assigned to the initial development of short range order in the 2D layers. This is followed by long range order at 3.3 K. Applied field measurements reveal the potential to induce magnetic transitions in moderately small fields of 2 T. Neutron powder diffraction enabled the determination of a unique magnetic space group P21'/c (#14.77) at 1.5 K. This magnetic structure consists of antiferromagnetically coupled Mn-Mn dimers with spins principally along the out of plane a-axis.

The dipolar-octupolar (DO) pyrochlores, R$_2$M$_2$O$_7$ (R = Ce, Sm, Nd), are key players in the search for realizable novel quantum spin liquid (QSL) states as a large parameter space within the DO pyrochlore phase diagram is theorized to host QSL states of both dipolar and octupolar nature. New single crystals and powders of Ce$_2$Sn$_2$O$_7$, synthesized by hydrothermal techniques, present an opportunity for a new characterization of the exchange parameters in Ce$_2$Sn$_2$O$_7$ using the near-neighbor $XYZ$ model Hamiltonian associated with DO pyrochlores. Utilizing quantum numerical linked cluster expansion fits to heat capacity and magnetic susceptibility measurements, and classical Monte Carlo calculations to the diffuse neutron diffraction of the new hydrothermally grown Ce$_2$Sn$_2$O$_7$ samples, we place Ce$_2$Sn$_2$O$_7$'s ground state within the ordered dipolar all-in-all-out (AIAO) N\'{e}el phase, with quantum Monte Carlo calculations showing a transition to long-range order at temperatures below those accessed experimentally. Indeed, our new neutron diffraction measurements on the hydrothermally grown Ce$_2$Sn$_2$O$_7$ powders show a broad signal at low scattering wave vectors, reminiscent of a \textit{dipolar} spin ice, in striking contrast from previous powder neutron diffraction on samples grown from solid-state synthesis, which found diffuse scattering at high scattering wave vectors associated with magnetic {\it octupoles} and suggested an octupolar quantum spin ice state. We conclude that new hydrothermally grown Ce$_2$Sn$_2$O$_7$ samples host a finite-temperature proximate dipolar spin ice phase, above the expected transition to AIAO N\'{e}el order., Comment: 16 pages, 12 figures

In this work, a temperature-induced valence-state transition is studied in a narrow composition range of Ba$_{2-x}$Sr$_x$TbIrO$_6$. The valence-state transition involves an electron transfer between Tb and Ir leading to the valence-state change between Tb$^{3+}$/Ir$^{5+}$ and Tb$^{4+}$/Ir$^{4+}$ phases. This first-order transition has a dramatic effect on the lattice, transport properties, and the long-range magnetic order at low temperatures for both Tb and Ir ions. Ir$^{5+}$ ion has an electronic configuration of 5$d^4$ ($J\rm_{eff}$ = 0) which is expected to be nonmagnetic. In contrast, Ir$^{4+}$ ion with a configuration of 5$d^5$($J\rm_{eff}$ = 1/2) favors a long-range magnetic order. For $x$ = 0.1 with Tb$^{3+}$/Ir$^{5+}$ configuration to the lowest temperature (2 K) investigated in this work, a spin-glass behavior is observed around 5 K indicating Ir$^{5+}$ ($J\rm_{eff}$ = 0) ions act as a spacer reducing the magnetic interactions between Tb$^{3+}$ ions. For $x$ = 0.5 with Tb$^{4+}$/Ir$^{4+}$ configuration below the highest temperature 400 K of this work, a long-range antiferromagnetic order at $T\rm_N$ = 40 K is observed highlighting the importance of Ir$^{4+}$ ($J\rm_{eff}$ = 1/2) ions in promoting the long-range magnetic order of both Tb and Ir ions. For 0.2 $\leqslant x \leqslant$ 0.375, a temperature-induced valence-state transition from high-temperature Tb$^{3+}$/Ir$^{5+}$ phase to low-temperature Tb$^{4+}$/Ir$^{4+}$ phase occurs in the temperature range 180 K $\leqslant T \leqslant$ 325 K and the transition temperature increases with $x$. The compositional dependence demonstrates the ability to tune the the valence state for a critical region of $x$ that leads to a concurrent change in magnetism and structure. This tuning ability could be employed with suitable strain in thin films to act as a switch as the magnetism is manipulated., Comment: 10 pages, 8 figures

Destructive interference of electron hopping on the frustrated kagome lattice generates Dirac nodes, saddle points, and flat bands in the electronic structure. The latter provides the narrow bands and a peak in the density of states that can generate correlated electron behavior when the Fermi level lies within them. In the kagome metal CoSn, this alignment is not realized, and the compound is a Pauli paramagnet. Here we show that replacing part of the tin with indium (CoSn1-xInx) moves the Fermi energy into the flat band region, with support from band structure calculations, heat capacity measurements, and angle resolved photoemission spectroscopy. The associated instability results in the emergence of itinerant antiferromagnetism with a Neel temperature up to 30K. Long range magnetic order is confirmed by neutron diffraction measurements, which indicate an ordered magnetic moment of 0.1-0.2 Bohr magnetons per Co (for x = 0.4). Thus, CoSn1-xInx provides a rare example of an itinerant antiferromagnet with a small ordered moment. This work provides clear evidence that flat bands arising from frustrated lattices in bulk crystals represent a viable route to new physics, evidenced here by the emergence of magnetic order upon introducing a non-magnetic dopant into a non-magnetic kagome metal.

We report a comprehensive investigation of Ln2NiIrO6 (Ln = La, Pr, Nd) using thermodynamic and transport properties, neutron powder diffraction, resonant inelastic x-ray scattering, and density functional theory (DFT) calculations to investigate the role of A-site cations on the magnetic interactions in this family of hybrid 3d-5d-4f compositions. Magnetic structure determination using neutron diffraction reveals antiferromagnetism for La2NiIrO6, a collinear ferrimagnetic Ni/Ir state that is driven to long range antiferromagnetism upon the onset of Nd ordering in Nd2NiIrO6, and a non-collinear ferrimagnetic Ni/Ir sublattice interpenetrated by a ferromagnetic Pr lattice for Pr2NiIrO6. For Pr2NiIrO6 heat capacity results reveal the presence of two independent magnetic sublattices and transport resistivity indicates insulating behavior and a conduction pathway that is thermally mediated. First principles DFT calculation elucidates the existence of the two independent magnetic sublattices within Pr2NiIrO6 and offers insight into the behavior in La2NiIrO6 and Nd2NiIrO6. Resonant inelastic x-ray scattering is consistent with spin-orbit coupling splitting the t2g manifold of octahedral Ir4+ into a Jeff = 1/2 and Jeff = 3/2 state for all members of the series considered.

Nd-based pyrochlore oxides of the form Nd$_{2}B_{2}$O$_{7}$ have garnered a significant amount of interest owing to the moment fragmentation physics observed in Nd$_{2}$Zr$_{2}$O$_{7}$ and speculated in Nd$_{2}$Hf$_{2}$O$_{7}$. Notably this phenomenon is not ubiquitous in this family, as it is absent in Nd$_{2}$Sn$_{2}$O$_{7}$, which features a smaller ionic radius on the $B$-site. Here, we explore the necessary conditions for moment fragmentation in the Nd pyrochlore family through a detailed study of the mixed $B$-site pyrochlore Nd$_{2}$GaSbO$_{7}$. The $B$-site of this system is characterized by significant disorder and an extremely small average ionic radius. Similarly to Nd$_{2}$Sn$_{2}$O$_{7}$, we find no evidence for moment fragmentation through our bulk characterization and neutron scattering experiments, indicating that chemical pressure (and not necessarily the $B$-site disorder) plays a key role in the presence or absence of this phenomenon in this material family. Surprisingly, the presence of significant $B$-site disorder in Nd$_{2}$GaSbO$_{7}$ does not generate a spin glass ground state and instead the same all-in-all-out magnetic order identified in other Nd pyrochlores is found here., Comment: 11 pages, 8 figures

We investigate the physical properties of the Shastry-Sutherland lattice material BaNd$_2$ZnO$_5$. Neutron diffraction, magnetic susceptibility, and specific heat measurements reveal antiferromagnetic order below 1.65 K. The magnetic order is found to be a 2-$\boldsymbol{Q}$ magnetic structure with the magnetic moments lying in the Shastry-Sutherland lattice planes comprising the tetragonal crystal structure of BaNd$_2$ZnO$_5$. The ordered moment for this structure is 1.9(1) $\mu_B$ per Nd ion. Inelastic neutron scattering measurements reveal that the crystal field ground state doublet is well separated from the first excited state at 8 meV. The crystal field Hamiltonian is determined through simultaneous refinement of models with both the LS coupling and intermediate coupling approximations to the inelastic neutron scattering and magnetic susceptibility data. The ground state doublet indicates that the magnetic moments lie primarily in the basal plane with magnitude consistent with the size of the determined ordered moment., Comment: 13 pages, 8 figures

Two-dimensional van der Waals compounds with magnetic ions on a honeycomb lattice are hosts to a variety of exotic behavior. The magnetic interactions in one such compound, MnPSe$_3$, are investigated with elastic and inelastic neutron scattering. Magnetic excitations are observed in the magnetically ordered regime and persist to temperatures well above the ordering temperature, $\rm T_N$ = 74 K, consistent with low dimensional magnetic interactions. The inelastic neutron scattering results allow a model spin Hamiltonian to be presented that includes dominant intralayer interactions of $J_{1ab}$=0.45 meV, $J_{2ab}$=0.03 meV, $J_{3ab}$=0.19 meV, and appreciable interlayer interactions of $J_c$=0.031(5) meV. No evidence for anisotropy in the form of a spin-gap is observed in the data collected. The measurements on MnPSe$_3$ are contrasted with those on MnPS$_3$ and reveal a large increase in the interlayer exchange interactions in MnPSe$_3$, despite the quasi-2D magnetic behavior.

We present a comprehensive experimental and theoretical study of the pyrochlore Tb$_2$Ge$_2$O$_7$, an exemplary realization of a material whose properties are dominated by competition between magnetic dipolar and electric quadrupolar correlations. The dipolar and quadrupolar correlations evolve over three distinct regimes that we characterize via heat capacity, elastic and inelastic neutron scattering. In the first regime, above $T^*=1.1$ K, significant quadrupolar correlations lead to an intense inelastic mode that cannot be accounted for within a scenario with solely magnetic dipole-dipole correlations. The onset of extended dipole correlations occurs in the intermediate regime, between $T^*=1.1$ K and $T_c = 0.25$ K, with the formation of a collective paramagnetic state characterized by extended ferromagnetic canted spin ice domains. Here, long-range order is impeded not only by the usual frustration operating in classical spin ice systems, but also by a competition between dipolar and quadrupolar correlations. Finally, in the lowest temperature regime, below $T_c=0.25$ K, there is an abrupt and significant increase in the dipole ordered moment. The majority of the ordered moment remains tied up in the ferromagnetic spin ice-like state, but an additional $\mathbf{k}=(0,0,1)$ antiferromagnetic order parameter also develops. Simultaneously, the spectral weight of the inelastic mode, which is a proxy for the quadrupolar correlations, is observed to drop, indicating that dipole order ultimately wins out. Tb$_2$Ge$_2$O$_7$ is therefore a remarkable platform to study intertwined dipolar and quadrupolar correlations in a magnetically frustrated system and provides important insights into the physics of the whole family of terbium pyrochlores.

Heavy transition metal magnets with $J_{\rm eff}$ $=$ 1/2 electronic ground states have attracted recent interest due to their penchant for hosting new classes of quantum spin liquids and superconductors. Unfortunately, model systems with ideal $J_{\rm eff}$ $=$ 1/2 states are scarce due to the importance of non-cubic local distortions in most candidate materials. In this work, we identify a family of iridium halide systems [i.e. K$_2$IrCl$_6$, K$_2$IrBr$_6$, (NH$_4$)$_2$IrCl$_6$, and Na$_2$IrCl$_6 \cdotp $ 6(H$_2$O)] with Ir$^{4+}$ electronic ground states in extremely close proximity to the ideal $J_{\rm eff}$ $=$ 1/2 limit, despite a variation in the low-temperature global crystal structures. We also find ordered magnetic ground states for the three anhydrous systems, with single crystal neutron diffraction on K$_2$IrBr$_6$ revealing Type-I antiferromagnetism. This spin configuration is consistent with expectations for significant Kitaev exchange in a face-centered-cubic magnet., Comment: 14 pages, 9 figures

Ising-like spin-1/2 magnetic materials are of interest for their ready connection to theory, particularly in the context of quantum critical behavior. In this work we report detailed studies of the magnetic properties of a member of the rare earth pyrosilicate family, D-Er$_{2}$Si$_{2}$O$_{7}$, which is known to display a highly anisotropic Ising-like g-tensor and effective spin-1/2 magnetic moments. We used powder neutron diffraction, powder inelastic neutron spectroscopy (INS), and single crystal AC susceptibility to characterize its magnetic properties. Neutron diffraction enabled us to determine the magnetic structure below the known transition temperature ($T_{N}$ = 1.9 K) in zero field, confirming that the magnetic state is a four-sublattice antiferromagnetic structure with two non-collinear Ising axes, as was previously hypothesized. Our powder INS data revealed a gapped excitation at zero field, consistent with anisotropic (possibly Ising) exchange. An applied field of 1 T produces a mode softening, which is consistent with a field-induced second order phase transition. To assess the relevance of D-Er$_{2}$Si$_{2}$O$_{7}$ to the transverse field Ising model, we performed AC susceptibility measurements on a single crystal with the magnetic field oriented in the direction transverse to the Ising axes. This revealed a transition at 2.65 T at 0.1 K, a field significantly higher than the mode-softening field observed by powder INS, showing that the field-induced phase transitions are highly field-direction dependent as expected. These measurements suggest that D-Er$_{2}$Si$_{2}$O$_{7}$ may be a candidate for further exploration related to the transverse field Ising model., Comment: AC suscep. data presented in the last version was incorrect. Revised with new data and conclusions

Compounds with two-dimensional (2D) layers of magnetic ions weakly connected by van der Waals bonding offer routes to enhance quantum behavior, stimulating both fundamental and applied interest. CrPS4 is one such magnetic van der Waals material, however, it has undergone only limited investigation. Here we present a comprehensive series of neutron scattering measurements to determine the magnetic structure and exchange interactions. The observed magnetic excitations allow a high degree of constraint on the model parameters not normally associated with measurements on a powder sample. The results demonstrate the 2D nature of the magnetic interactions, while also revealing the importance of interactions along 1D chains within the layers. The subtle role of competing interactions is observed, which manifest in a non-trivial magnetic transition and a tunable magnetic structure in a small applied magnetic field through a spin-flop transition. Our results on the bulk compound provide insights that can be applied to an understanding of the behavior of reduced layer CrPS4.

Molecular magnets based on heavy transition metals have recently attracted significant interest in the quest for novel magnetic properties. For systems with an odd number of valence electrons per molecule, high or low molecular spin states are typically expected in the double exchange or quasi-molecular orbital limits respectively. In this work, we use bulk characterization, muon spin relaxation, neutron diffraction, and inelastic neutron scattering to identify a rare intermediate spin-3/2 per dimer state in the 6H-perovskite Ba$_3$LaRu$_2$O$_9$ that cannot be understood in a double exchange or quasi-molecular orbital picture and instead arises from orbital-selective Mott insulating behavior at the molecular level. Our measurements are also indicative of collinear stripe magnetic order below $T_N$ = 26(1) K for these molecular spin-3/2 degrees-of-freedom, which is consistent with expectations for an ideal triangular lattice with significant next nearest neighbor in-plane exchange. Finally, we present neutron diffraction and Raman scattering data under applied pressure that reveal low-lying structural and spin state transitions at modest pressures P $\le$ 1 GPa, which highlights the delicate balance between competing energy scales in this system., Comment: 12 pages, 10 figures

We report for the first time the magnetic structure of the high entropy oxide $(Mg_{0.2}Co_{0.2}Ni_{0.2}Cu_{0.2}Zn_{0.2})O$ using neutron powder diffraction. This material exhibits a sluggish magnetic transition but possesses a long-range ordered antiferromagnetic ground state, as revealed by DC and AC magnetic susceptibility, elastic and inelastic neutron scattering measurements. The magnetic propagation wavevector is k=(1/2, 1/2, 1/2) based on the cubic structure Fm-3m, and the magnetic structure consists of ferromagnetic sheets in the (111) planes with spins antiparallel between two neighboring planes. Inelastic neutron scattering reveals strong magnetic excitations at 100 K that survive up to room temperature. This work demonstrates that entropy-stabilized oxides represent a unique platform to study long range magnetic order with extreme chemical disorder., Comment: 13 pages, 4 figures, supplemental material is upon request

Quantum magnets with significant bond-directional Ising interactions, so-called Kitaev materials, have attracted tremendous attention recently in the search for exotic spin liquid states. Here we present a comprehensive set of measurements that enables us to investigate the crystal structures, Ir$^{4+}$ single ion properties, and magnetic ground states of the double perovskite iridates La$_2B$IrO$_6$ ($B$ $=$ Mg, Zn) and $A_2$CeIrO$_6$ ($A$ $=$ Ba, Sr) with a large nearest neighbor distance $>$ 5 Angstroms between Ir$^{4+}$ ions. Our neutron powder diffraction data on Ba$_2$CeIrO$_6$ can be refined in the cubic space group Fm$\bar{3}$m, while the other three systems are characterized by weak monoclinic structural distortions. Despite the variance in the non-cubic crystal field experienced by the Ir$^{4+}$ ions in these materials, X-ray absorption spectroscopy and resonant inelastic x-ray scattering are consistent with $J_{\rm eff}$ $=$ 1/2 moments in all cases. Furthermore, neutron scattering and resonant magnetic x-ray scattering show that these systems host A-type antiferromagnetic order. These electronic and magnetic ground states are consistent with expectations for face-centered-cubic magnets with significant antiferromagnetic Kitaev exchange, which indicates that spacing magnetic ions far apart may be a promising design principle for uncovering additional Kitaev materials., Comment: 12 pages, 7 figures

High-resolution resonant inelastic x-ray scattering (RIXS) measurements ($\Delta$E = 46 meV) have been performed on Cd$_2$Os$_2$O$_7$ through the metal-to-insulator transition (MIT). A magnetic excitation at 125 meV evolves continuously through the MIT, in agreement with recent Raman scattering results, and provides further confirmation for an all-in, all-out magnetic ground state. Asymmetry of this feature is likely a result of coupling between the electronic and magnetic degrees of freedom. We also observe a broad continuum of interband excitations centered at 0.3 eV energy loss. This is indicative of significant hybridization between Os 5$d$ and O 2$p$ states, and concurrent itinerant nature of the system. In turn, this suggests a possible break down of the free-ion model for Cd$_2$Os$_2$O$_7$., Comment: Accepted in Physical Review B (10 pages)

Fe3-xGeTe2 is an itinerant ferromagnet composed of two-dimensional layers weakly connected by van der Waals bonding that shows a variety of intriguing phenomena. Inelastic neutron scattering measurements on bulk single crystals of Fe2.75GeTe2 were performed to quantify the magnetic exchange interaction energies and anisotropy. The observed inelastic excitations are indicative of dominant in-plane correlations with negligible magnetic interactions between the layers. A spin-gap of 3.9 meV is observed allowing a measure of the magnetic anisotropy. As the excitations disperse to their maximum energy (~65 meV) they become highly damped, reflective of both the magnetic site occupancy reduction of 25{\%} on one Fe sublattice and the itinerant interactions. A minimal model is employed to describe the excitation spectra and extract nearest neighbor magnetic exchange interaction values. The temperature evolution of the excitations are probed and correlations shown to persist above Tc, indicative of low dimensional magnetism.

Time-of-flight inelastic neutron scattering measurements on Sr2IrO4 single crystals were performed to access the spin Hamiltonian in this canonical Jeff=1/2 spin-orbital Mott insulator. The momentum of magnetic scattering at all inelastic energies that were measured is revealed to be $L$-independent, indicative of idealized two-dimensional in-plane correlations. By probing the in-plane energy and momentum dependence up to ~80 meV we model the magnetic excitations and define a spin-gap of 0.6(1) meV. Collectively the results indicate that despite the strong spin-orbit entangled isospins an isotropic two-dimensional S=1/2 Heisenberg model Hamiltonian accurately describes the magnetic interactions, pointing to a robust analogy with unconventional superconducting cuprates.

In frustrated spinel antiferromagnets, dilution with non-magnetic ions can be a powerful strategy for probing unconventional spin states or uncovering interesting phenomena. Here, we present X-ray, neutron scattering and thermodynamic studies of the effects of magnetic dilution of the tetragonally-distorted A-site spinel antiferromagnet, CuRh$_2$O$_4$, with non-magnetic Zn$^{2+}$ ions. Our data confirm the helical spin order recently identified at low-temperatures in this material, and further demonstrate a systematic suppression of the associated N\'eel temperature with increasing site dilution towards a continuous transition with critical doping of $x_{spin} \sim 0.44$. Interestingly, this critical doping is demonstrably distinct from a second structural critical point at $x_{JT} \sim 0.6$, which is consistent with the suppression of orbital order on the A-site through a classical percolative mechanism. This anomalously low value for $x_{spin}$ is confirmed via multiple measurements, and is inconsistent with predictions of classical percolation theory, suggesting that the spin transition in this material is driven by an enhancement of pre-existing spin fluctuations with weak dilution., Comment: 9 pages, 5 figures

Sr$_2$FeOsO$_6$ is an insulating double perovskite compound which undergoes antiferromagnetic transitions at 140 K ($T_{N1}$) and 67 K ($T_{N2}$). To study the underlying electronic and magnetic interactions giving rise to this behavior we have performed inelastic neutron scattering (INS) and resonant inelastic x-ray scattering (RIXS) experiments on polycrystalline samples of Sr$_2$FeOsO$_6$. The INS data reveal that the spectrum of spin excitations remains ungapped below T$_{N1}$, however below T$_{N2}$ a gap of 6.8 meV develops. The RIXS data reveals splitting of the T$_{2g}$ multiplet consistent with that seen in other 5d$^3$ osmium based double perovskites. Together these results suggest that spin-orbit coupling is important for ground state selection in 3d-5d$^3$ double perovskite materials., Comment: 5 figures, supplementary material available on request

The physical properties of the spinel LiGaCr4S8 have been studied with neutron diffraction, X-ray diffraction, magnetic susceptibility and heat capacity measurements. The neutron diffraction and synchrotron X-ray diffraction data reveal negative thermal expansion (NTE) below 111(4) K. The magnetic susceptibility deviates from Curie-Weiss behavior with the onset of NTE. At low temperature a broad peak in the magnetic susceptibility at 10.3(3) K is accompanied by the return of normal thermal expansion. First principles calculations find a strong coupling between the lattice and the simulated magnetic ground state. These results indicate strong magnetoelastic coupling in LiGaCr4S8.

The electronic ground state of Ca3LiOsO6 was recently considered within an intermediate coupling regime that revealed J=3/2 spin-orbit entangled magnetic moments. Through inelastic neutron scattering and density functional theory we investigate the magnetic interactions and probe how the magnetism is influenced by the change in hierarchy of interactions as we move from Ca3LiOsO6 (5d3) to Ca3LiRuO6 (4d3). An alteration of the spin-gap and ordered local moment is observed, however the magnetic structure, Neel temperature and exchange interactions are unaltered. To explain this behavior it is necessary to include both spin-orbit coupling and hybridization, indicating the importance of an intermediate coupling approach when describing 5$d$ oxides.

Magnetic monopoles are hypothesised elementary particles connected by Dirac strings that behave like infinitely thin solenoids. Despite decades of searches, free magnetic monopoles and their Dirac strings have eluded experimental detection, although there is substantial evidence for deconfined magnetic monopole quasiparticles in spin ice materials. Here we report the detection of a hierarchy of unequally-spaced magnetic excitations \emph{via} high resolution inelastic neutron spectroscopic measurements on the quantum spin ice candidate Pr$_{2}$Sn$_{2}$O$_{7}$. These excitations are well-described by a simple model of monopole pairs bound by a linear potential with an effective tension of 0.642(8) K~$\cdot$\AA$^{-1}$ at 1.65~K. The success of the linear potential model suggests that these low energy magnetic excitations are direct spectroscopic evidence for the confinement of magnetic monopole quasiparticles in the quantum spin ice candidate Pr$_{2}$Sn$_{2}$O$_{7}$., Comment: 9 pages, 4 figures

The perovskite SrIrO3 is an exotic narrow-band metal owing to a confluence of the strengths of the spin-orbit coupling (SOC) and the electron-electron correlations. It has been proposed that topological and magnetic insulating phases can be achieved by tuning the SOC, Hubbard interactions, and/or lattice symmetry. Here, we report that the substitution of nonmagnetic, isovalent Sn4+ for Ir4+ in the SrIr1-xSnxO3 perovskites synthesized under high pressure leads to a metal-insulator transition to an antiferromagnetic (AF) phase at TN > 225 K. The continuous change of the cell volume as detected by x-ray diffraction and the lamda-shape transition of the specific heat on cooling through TN demonstrate that the metal-insulator transition is of second-order. Neutron powder diffraction results indicate that the Sn substitution enlarges an octahedral-site distortion that reduces the SOC relative to the spin-spin exchange interaction and results in the type-G AF spin ordering below TN. Measurement of high-temperature magnetic susceptibility shows the evolution of magnetic coupling in the paramagnetic phase typical of weak itinerant-electron magnetism in the Sn-substituted samples. A reduced structural symmetry in the magnetically ordered phase leads to an electron gap opening at the Brillouin zone boundary below TN in the same way as proposed by Slater., Comment: 15 pages, 4 figures

The insulating magnetic material Fe3PO4O3 features a non-centrosymmetric lattice composed of Fe^{3+} triangular units. Frustration, due to competing near neighbor ($J_1$) and next nearest neighbor ($J_2$) antiferromagnetic interactions, was recently suggested to be the origin of an antiferromagnetic helical ground state with unusual needle-like nanoscale magnetic domains in Fe3PO4O3. Magnetic dilution is shown here to tune the ratio of these magnetic interactions, thus providing deeper insight into this unconventional antiferromagnet. Dilution of the Fe^{3+} lattice in Fe3PO4O3 was accomplished by substituting non-magnetic Ga^{3+} to form the solid solution series Fe_{3-x}Ga_xPO4O3 with $x = 0.012, 0.06, 0.25, 0.5, 1.0, 1.5$. Magnetic susceptibility and neutron powder diffraction data from this series are presented. A continuous decrease of the both the helical pitch length and the domain size is observed with increasing dilution up to at least $x = 0.25$, while for $x \ge 0.5$, the compounds lack long range magnetic order entirely. The decrease in the helical pitch length with increasing $x$ can be qualitatively understood by reduction of the ratio of $J_2/J_1$ in the Heisenberg model, consistent with mean field considerations. Intriguingly, the magnetic correlation length in the $ab$ plane remains nearly equal to the pitch length for each value of $x \le 0.25$, showing that the two quantities are intrinsically connected in this unusual antiferromagnet., Comment: 8 pages, 7 figures

The layered perovskites $R$Cr(BO$_3$)$_2$ ($R$ = Y and Ho) with magnetic triangular lattices were studied by performing ac/dc susceptibility, specific heat, elastic and inelastic neutron scattering, and dielectric constant measurements. The results show (i) both samples' Cr$^{3+}$ spins order in a canted antiferromagnetic structure with $T_N$ around 8-9 K, while the Ho$^{3+}$ ions do not order down to $T$ = 1.5 K in HoCr(BO$_3$)$_2$; (ii) when a critical magnetic field H$_{C}$ around 2-3 T is applied below $T_{N}$, the Cr$^{3+}$ spins in the Y-compound and both the Cr$^{3+}$ and Ho$^{3+}$ spins in the Ho-compound order in a ferromagnetic state; (iii) both samples exhibit dielectric constant anomalies around the transition temperature and critical field, but the Ho-compound displays a much stronger magnetodielectric response. We speculate that this is due to the magnetostriction which depends on both of the Cr$^{3+}$ and the Ho$^{3+}$ ions' ordering in the Ho-compound. Moreover, by using linear spin wave theory to simulate the inelastic neutron scattering data, we estimated the Y-compound's intralayer and interlayer exchange strengths as ferromagnetic J$_{1}$ = -0.12 meV and antiferromagnetic J$_{2}$ = 0.014 meV, respectively. The competition between different kinds of superexchange interactions results in the ferromagnetic intralayer interaction., Comment: 11 pages, 12 figures

NaOsO$_{\text{3}}$ undergoes a metal-insulator transition (MIT) at 410 K, concomitant with the onset of antiferromagnetic order. The excitation spectra have been investigated through the MIT by resonant inelastic x-ray scattering (RIXS) at the Os L$_{\text{3}}$ edge. Low resolution ($\Delta E \sim$ 300 meV) measurements over a wide range of energies reveal that local electronic excitations do not change appreciably through the MIT. This is consistent with a picture in which structural distortions do not drive the MIT. In contrast, high resolution ($\Delta E \sim $ 56 meV) measurements show that the well-defined, low energy magnons in the insulating state weaken and dampen upon approaching the metallic state. Concomitantly, a broad continuum of excitations develops which is well described by the magnetic fluctuations of a nearly antiferromagnetic Fermi liquid. By revealing the continuous evolution of the magnetic quasiparticle spectrum as it changes its character from itinerant to localized, our results provide unprecedented insight into the nature of the MIT in \naoso. In particular, the presence of weak correlations in the paramagnetic phase implies a degree of departure from the ideal Slater limit., Comment: Joint submission with Physical Review Letters [Phys. Rev. Lett. 120, 227203 (2018), accepted version at arXiv:1805.03176]. This article includes further discussion about the calculations performed, models used, and so on

Antiferromagnetic insulators on the diamond lattice are candidate materials to host exotic magnetic phenomena ranging from spin-orbital entanglement to degenerate spiral ground-states and topological paramagnetism. Compared to other three-dimensional networks of magnetic ions, such as the geometrically frustrated pyrochlore lattice, the investigation of diamond-lattice magnetism in real materials is less mature. In this work, we characterize the magnetic properties of model A-site spinels CoRh2O4 (cobalt rhodite) and CuRh2O4 (copper rhodite) by means of thermo-magnetic and neutron scattering measurements and perform group theory analysis, Rietveld refinement, mean-field theory, and spin wave theory calculations to analyze the experimental results. Our investigation reveals that cubic CoRh2O4 is a canonical S=3/2 diamond-lattice Heisenberg antiferromagnet with a nearest neighbor exchange J = 0.63 meV and a Neel ordered ground-state below a temperature of 25 K. In tetragonally distorted CuRh2O4, competiting exchange interactions between up to third nearest-neighbor spins lead to the development of an incommensurate spin helix at 24 K with a magnetic propagation vector k = (0,0,0.79). Strong reduction of the ordered moment is observed for the S=1/2 spins in CuRh2O4 and captured by our 1/S corrections to the staggered magnetization. Our work identifies CoRh2O4 and CuRh2O4 as reference materials to guide future work searching for exotic quantum behavior in diamond-lattice antiferromagnets., Comment: 15 pages, 14 figures

To understand emergent magnetic monopole dynamics in the spin ices Ho$_2$Ti$_2$O$_7$ and Dy$_2$Ti$_2$O$_7$, it is necessary to investigate the mechanisms by which spins flip in these materials. Presently there are thought to be two processes: quantum tunneling at low and intermediate temperatures and thermally activated at high temperatures. We identify possible couplings between crystal field and optical phonon excitations and construct a strictly constrained model of phonon-mediated spin flipping that quantitatively describes the high-temperature processes in both compounds, as measured by quasielastic neutron scattering. We support the model with direct experimental evidence of the coupling between crystal field states and optical phonons in Ho$_2$Ti$_2$O$_7$.

The dispersive magnetic excitations in Sr2IrO4 have previously been well described within an isospin-1/2 Heisenberg model on a square lattice that revealed parallels with La2CuO4. Here we investigate the inelastic spectra of Sr2Ir0.8Ru0.2O4 with resonant inelastic x-ray scattering (RIXS) at the Ir L3-edge. The results are well described using linear spin-wave theory within a similar Heisenberg model applicable to Sr2IrO4, however the disorder induced by the substitution of 20% Ir4+ ions for Ru4+ removes longer range exchange interactions. A large spin-gap (40 meV) is measured indicating strong anisotropy from spin-orbit coupling that is manifest due to the altered magnetic structure in Sr2Ir0.8Ru0.2O4 with c-axis aligned moments compared to the basal plane moments in the parent. Collectively the results indicate the robustness of a Heisenberg model description even when the magnetic structure is altered and the J=1/2 moments diluted.

Entanglement of spin and orbital degrees of freedom drives the formation of novel quantum and topological physical states. Discovering new spin-orbit entangled ground states and emergent phases of matter requires both experimentally probing the relevant energy scales and applying suitable theoretical models. Here we report resonant inelastic x-ray scattering measurements of the transition metal oxides Ca$_3$LiOsO$_6$ and Ba$_2$YOsO$_6$. We invoke an intermediate coupling approach that incorporates both spin-orbit coupling and electron-electron interactions on an even footing and reveal the ground state of $5d^3$ based compounds, which has remained elusive in previously applied models, is a novel spin-orbit entangled J=3/2 electronic ground state. This work reveals the hidden diversity of spin-orbit controlled ground states in 5d systems and introduces a new arena in the search for spin-orbit controlled phases of matter., Comment: main text plus supplemental information

NaOsO3 hosts a rare manifestation of a metal-insulator transition driven by magnetic correlations, placing the magnetic exchange interactions in a central role. We use resonant inelastic x-ray scattering to directly probe these magnetic exchange interactions. A dispersive and strongly gapped (58 meV) excitation is observed indicating appreciable spin-orbit coupling in this 5d3 system. The excitation is well described within a minimal model Hamiltonian with strong anisotropy and Heisenberg exchange (J1=J2=13.9 meV). The observed behavior places NaOsO3 on the boundary between localized and itinerant magnetism.

The structural properties of LaCu$_{6-x}$Au$_x$ have been studied using neutron diffraction, x-ray diffraction, and heat capacity measurements. The continuous orthorhombic-monoclinic structural phase transition in LaCu$_{6}$ is suppressed linearly with Au substitution until a complete suppression of the structural phase transition occurs at the critical composition, $x_{c}$ = 0.3. Heat capacity measurements at low temperatures indicate residual structural instability at $x_c$ that extends well into the orthorhombic phase. The instability is ferroelastic in nature, with density functional theory (DFT) calculations showing negligible coupling to electronic states near the Fermi level. The data and calculations presented here are consistent with the zero temperature termination of a continuous structural phase transition suggesting that the LaCu$_{6-x}$Au$_x$ series hosts an elastic quantum critical point., Comment: 9 pages, 11 figures

We have performed inelastic neutron scattering (INS) experiments to investigate the magnetic excitations in the weakly distorted face-centered-cubic (fcc) iridate double perovskites La$_2$ZnIrO$_6$ and La$_2$MgIrO$_6$, which are characterized by A-type antiferromagnetic ground states. The powder inelastic neutron scattering data on these geometrically frustrated $j_{\rm eff}=1/2$ Mott insulators provide clear evidence for gapped spin wave excitations with very weak dispersion. The INS results and thermodynamic data on these materials can be reproduced by conventional Heisenberg-Ising models with significant uniaxial Ising anisotropy and sizeable second-neighbor ferromagnetic interactions. Such a uniaxial Ising exchange interaction is symmetry-forbidden on the ideal fcc lattice, so that it can only arise from the weak crystal distortions away from the ideal fcc limit. This may suggest that even weak distortions in $j_{\rm eff}=1/2$ Mott insulators might lead to strong exchange anisotropies. More tantalizingly, however, we find an alternative viable explanation of the INS results in terms of spin models with a dominant Kitaev interaction. In contrast to the uniaxial Ising exchange, the highly-directional Kitaev interaction is a type of exchange anisotropy which is symmetry-allowed even on the ideal fcc lattice. The Kitaev model has a magnon gap induced by quantum order-by-disorder, while weak anisotropies of the Kitaev couplings generated by the symmetry-lowering due to lattice distortions, can pin the order and enhance the magnon gap. Our findings highlight how even conventional magnetic orders in heavy transition metal oxides may be driven by highly-directional exchange interactions rooted in strong spin-orbit coupling., Comment: 11 pages, 5 figures. arXiv admin note: text overlap with arXiv:1507.07920

The singlet ground state magnetism in pyrochlore osmates Y$_2$Os$_2$O$_7$ and Ho$_2$Os$_2$O$_7$ is studied by DC and AC susceptibility, specific heat, and neutron powder diffraction measurements. Despite the expected non-magnetic singlet in the strong spin-orbit coupling (SOC) limit for Os$^{4+}$ ($5d^4$), Y$_2$Os$_2$O$_7$ exhibits a spin-glass (SG) ground state below 4 K with weak magnetism, suggesting possible proximity to a quantum phase transition between the non-magnetic state in the strong SOC limit and the magnetic state in the strong superexchange limit. Ho$_2$Os$_2$O$_7$ has the same structural distortion as occurs in Y$_2$Os$_2$O$_7$. However, the Os sublattice in Ho$_2$Os$_2$O$_7$ shows long-range magnetic ordering below 36\,K. The sharp difference of the magnetic ground state between Y$_2$Os$_2$O$_7$ and Ho$_2$Os$_2$O$_7$ signals the singlet ground state magnetism in $R_2$Os$_2$O$_7$ is fragile and can be disturbed by the weak $4f-5d$ interactions., Comment: 7 pages, 6 figures

We have performed magnetic susceptibility, heat capacity, neutron powder diffraction, and muon spin relaxation experiments to investigate the magnetic ground states of the 5$d^2$ double perovskites Sr$_2$YReO$_6$ and Sr$_2$InReO$_6$. We find that Sr$_2$YReO$_6$ is a spin glass, while Sr$_2$InReO$_6$ hosts a non-magnetic singlet state. By making detailed comparisons with other 5$d^2$ double perovskites, we argue that a delicate interplay between spin-orbit coupling, non-cubic crystal fields, and exchange interactions plays a key role in the great variation of magnetic ground states observed for this family of materials., Comment: 10 pages, 7 figures, submitted to PRB

The unusual magnetic and electronic ground states of 5d iridates has been shown to be driven by intrinsically enhanced spin-orbit coupling (SOC). The influence of appreciable but reduced SOC in creating the manifested magnetic insulating states in 4d oxides is less clear, with one hurdle being the existence of such compounds. Here we present experimental and theoretical results on Sr$_4$RhO$_6$ that reveal SOC dominated behavior. Neutron measurements show the octahedra are both spatially separated and locally ideal, making the electronic ground state susceptible to alterations by SOC. Magnetic ordering is observed with a similar structure to an analogous ${J}_{\mathrm{eff}}\mathbf{=}1/2$ Mott iridate. We consider the underlying role of SOC in this rhodate with density functional theory and x-ray absorption spectroscopy and find a magnetic insulating ground state with ${J}_{\mathrm{eff}}\mathbf{=}1/2$ character.

We report neutron scattering experiments which reveal a large spin gap in the magnetic excitation spectrum of weakly-monoclinic double perovskite Sr2ScOsO6. The spin gap is demonstrative of appreciable spin-orbit-induced anisotropy, despite nominally orbitally-quenched 5d3 Os5+ ions. The system is successfully modeled including nearest neighbor interactions in a Heisenberg Hamiltonian with exchange anisotropy. We find that the presence of the spin-orbit-induced anisotropy is essential for the realization of the type I antiferromagnetic ground state. This demonstrates that physics beyond the LS or JJ coupling limits plays an active role in determining the collective properties of 4d3 and 5d3 systems, and that theoretical treatments must include spin-orbit coupling., Comment: 6 pages, 4 figures, 4 pages supplementary material

The structural and the magnetic properties of CeCu$_{6-x}$Ag$_x$ (0 $\leq$ $x$ $\leq$ 0.85) and CeCu$_{6-x}$Pd$_x$ (0 $\leq$ $x$ $\leq$ 0.4) have been studied using neutron diffraction, resonant ultrasound spectroscopy (RUS), heat capacity, x-ray diffraction measurements and first principles calculations. The structural and magnetic phase diagrams of CeCu$_{6-x}$Ag$_x$ and CeCu$_{6-x}$Pd$_x$ as a function of Ag/Pd composition are reported. The end member, CeCu$_6$, undergoes a structural phase transition from an orthorhombic ($Pnma$) to a monoclinic ($P2_1/c$) phase at 240 K. In CeCu$_{6-x}$Ag$_x$, the structural phase transition temperature (${T_{s}}$) decreases linearly with Ag concentration and extrapolates to zero at $x_{S}$ $\approx$ 0.1. The structural transition in CeCu$_{6-x}$Pd$_x$ remains unperturbed with Pd substitution within the range of our study. The lattice constant $b$ slightly decreases with Ag/Pd doping, whereas, $a$ and $c$ increase with an overall increase in the unit cell volume. Both systems, CeCu$_{6-x}$Ag$_x$ and CeCu$_{6-x}$Pd$_x$, exhibit a magnetic quantum critical point (QCP), at $x$ $\approx$ 0.2 and $x$ $\approx$ 0.05 respectively. Near the QCP, long range antiferromagnetic ordering takes place at an incommensurate wave vector ($\delta_1$ 0 $\delta_2$) where $\delta_1 \sim 0.62$, $\delta_2 \sim 0.25$, $x$ = 0.125 for CeCu$_{6-x}$Pd$_x$ and $\delta_1 \sim 0.64$, $\delta_2 \sim 0.3$, $x$ = 0.3 for CeCu$_{6-x}$Ag$_x$. The magnetic structure consists of an amplitude modulation of the Ce-moments which are aligned along the $c$-axis of the orthorhombic unit cell., Comment: 13 pages, 9 figures

The rich physics manifested by 5d oxides falls outside the Mott-Hubbard paradigm used to successfully explain the electronic and magnetic properties of 3d oxides. Much consideration has been given to the extent to which strong spin-orbit coupling (SOC), in the limit of increased bandwidth and reduced electron correlation, drives the formation of novel electronic states, as manifested through the existence of metal-insulator transitions (MITs). SOC is believed to play a dominant role in 5d5 systems such as iridates (Ir4+), undergoing MITs which may or may not be intimately connected to magnetic order, with pyrochlore and perovksite systems being examples of the former and latter, respectively. However, the role of SOC for other 5d configurations is less clear. For example, 5d3 (e.g Os5+) systems are expected to have an orbital singlet and consequently a reduced effect of SOC in the groundstate. The pyrochlore osmate Cd2Os2O7 nonetheless exhibits a MIT intimately entwined with magnetic order with phenomena similar to pyrochlore iridates. Here we report the first resonant inelastic X-ray scattering (RIXS) measurements on an osmium compound, allowing us to determine the salient electronic and magnetic energy scales controlling the MIT in Cd2Os2O7, which we benchmark against detailed quantum chemistry calculations. In particular, we reveal the emergence at the MIT of a magnetic excitation corresponding to a superposition of multiple spin-flip processes from an Ising-like all-in/all-out magnetic groundstate. We discuss our results with respect to the role of SOC in magnetically mediated MITs in 5d systems

We investigate the magnetic properties of the series Sr2Ir1-xRuxO4 with neutron, resonant x-ray and magnetization measurements. The results indicate an evolution and coexistence of magnetic structures via a spin flop transition from ab-plane to c-axis collinear order as the 5d Ir4+ ions are replaced with an increasing concentration of 4d Ru4+ ions. The magnetic structures within the ordered regime of the phase diagram (x<0.3) are reported. Despite the changes in magnetic structure no alteration of the Jeff=1/2 ground state is observed. The behavior of Sr2Ir1-xRuxO4 is consistent with electronic phase separation and diverges from a standard scenario of hole doping. The role of lattice alterations with doping on the magnetic and insulating behavior is considered. The results presented here provide insight into the magnetic insulating states in strong spin-orbit coupled materials and the role perturbations play in altering the behavior.

We have performed inelastic neutron scattering experiments to investigate the magnetic excitations in the quasi-face-centered-cubic (fcc) iridate double perovskites La2ZnIrO6 and La2MgIrO6, which are characterized by A-type antiferromagnetic ground states. The neutron scattering data, which reveal gapped spin wave excitations with a very weak dispersion, are shown to be well-described by theoretical calculations on a model Hamiltonian with dominant Kitaev interactions. Our surprising finding shows that in contrast to honeycomb materials, where the Kitaev interaction manifests itself via complex magnetic order, even conventional magnetic orders in certain geometrically frustrated systems might owe their existence to unconventional Kitaev exchange., Comment: Superseded by significantly extended version with additional data+theory --- http://arxiv.org/abs/1604.08431

We report elastic and inelastic neutron scattering measurements of the high-TC ferromagnet Mn(1+delta)Sb. Measurements were performed on a large, TC=434 K, single crystal with interstitial Mn content of delta~0.13. The neutron diffraction results reveal that the interstitial Mn has a magnetic moment, and that it is aligned antiparallel to the main Mn moment. We perform density functional theory calculations including the interstitial Mn, and find the interstitial to be magnetic in agreement with the diffraction data. The inelastic neutron scattering measurements reveal two features in the magnetic dynamics: i) a spin-wave-like dispersion emanating from ferromagnetic Bragg positions (H K 2n), and ii) a broad, non-dispersive signal centered at forbidden Bragg positions (H$\,$K$\,$2$n$+1). The inelastic spectrum cannot be modeled by simple linear spin-wave theory calculations, and appears to be significantly altered by the presence of the interstitial Mn ions. The results show that the influence of the interstitial Mn on the magnetic state in this system is more important than previously understood., Comment: 11 pages, 10 figures, accepted to Physical Review B

We have investigated the magnetic ground state of the antiferromagnetic Kondo-lattice compounds CeMAl$_{4}$Si$_{2}$ (M = Rh, Ir) using neutron powder diffraction. Although both of these compounds show two magnetic transitions $T_{N1}$ and $T_{N2}$ in the bulk properties measurements, evidence for magnetic long-range order was only found below the lower transition $T_{N2}$. Analysis of the diffraction profiles reveals a commensurate antiferromagnetic structure with a propagation vector $\mathbf{k}$= (0, 0, 1/2). The magnetic moment in the ordered state of CeRhAl$_{4}$Si$_{2}$ and CeIrAl$_{4}$Si$_{2}$ were determined to be 1.14(2) and 1.41(3) $\mu_{B}$/Ce, respectively, and are parallel to the crystallographic $c$-axis in agreement with magnetic susceptibility measurements.

The magnetic susceptibility, crystal and magnetic structures, and electronic structure of double perovskite Sr2ScOsO6 are reported. Using both neutron and x-ray powder diffraction we find that the crystal structure is monoclinic P21/n from 3.5 to 300 K. Magnetization measurements indicate an antiferromagnetic transition at TN=92K, one of the highest transition temperatures of any double perovskite hosting only one magnetic ion. Type I antiferromagnetic order is determined by neutron powder diffraction, with an Os moment of only 1.6(1) muB, close to half the spin-only value for a crystal field split 5d electron state with t2g^3 ground state. Density functional calculations show that this reduction is largely the result of strong Os-O hybridization, with spin-orbit coupling responsible for only a ~0.1 muB reduction in the moment., Comment: 5 pages, 4 figures

Enhanced coupling of material properties offers new fundamental insights and routes to multifunctional devices. In this context 5d oxides provide new paradigms of cooperative interactions driving novel emergent behavior. This is exemplified in 5d osmates that host a metal-insulator transition (MIT) driven by magnetic order. Here we consider the most robust case, the 5d perovskite NaOsO3, and reveal a giant coupling between spin and phonon through a frequency shift of {\Delta}{\omega}=40 cm-1, the largest measured in any material. We identify the dominant octahedral breathing mode and show isosymmetry with spin ordering which induces dynamic charge disproportionation that sheds new light on the MIT. The occurrence of the dramatic spin-phonon-electronic coupling in NaOsO3 is due to a property common to all 5d materials: the large spatial extent of the 5d ion. This allows magnetism to couple to phonons on an unprecedented scale and consequently offers multiple new routes to enhanced coupled phenomena.