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Register a new userCoupled Spin-Charge-Phonon Fluctuation in the All-In/All-Out Antiferromagnet Cd$_2$Os$_2$O$_7$
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We report on a novel spin-charge fluctuation in the all-in-all-out pyrochlore magnet Cd$_2$Os$_2$O$_7$, where the spin fluctuation is driven by the conduction of thermally excited electrons/holes and associated fluctuation of Os valence. The fluctuation exhibits an activation energy significantly greater than the spin-charge excitation gap and a peculiar frequency range of $10^{6}$--$10^{10}$ s$^{-1}$. These features are attributed to the hopping motion of carriers as small polarons in the insulating phase, where the polaron state is presumably induced by the magnetoelastic coupling via the strong spin-orbit interaction. Such a coupled spin-charge-phonon fluctuation manifests as a part of the metal-insulator transition that is extended over a wide temperature range due to the modest electron correlation comparable with other interactions characteristic for 5$d$-subshell systems.
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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$_7$.
Dimensionality and symmetry play deterministic roles in the laws of Nature. They are important tools to characterize and understand quantum phase transitions, especially in the limit of strong correlations between spin, orbit, charge, and structural degrees of freedom. Using newly-developed, high-pressure resonant x-ray magnetic and charge diffraction techniques, we have discovered a quantum critical point in Cd2Os2O7 as the all-in-all-out (AIAO) antiferromagnetic order is continuously suppressed to zero temperature and, concomitantly, the cubic lattice structure continuously changes from space group Fd-3m to F-43m. Surrounded by three phases of different time reversal and spatial inversion symmetries, the quantum critical region anchors two phase lines of opposite curvature, with striking departures from a mean-field form at high pressure. As spin fluctuations, lattice breathing modes, and quasiparticle excitations interact in the quantum critical region, we argue that they present the necessary components for strongly-coupled quantum criticality in this three-dimensional compound.
The XY-pyrochlore antiferromagnet ETO is studied by heat capacity measurements and electron spin resonance spectroscopy performed on single crystal samples. The magnetic phase diagrams are established for two directions of applied field, $Hparallel [100]$ and $Hparallel [111]$. In the magnetically ordered phase observed below $T_N=1.2$ K, the magnetic excitation spectrum consists of a Goldstone mode acquiring an isotropic gap in an applied field, and another mode with a gap softening in the vicinity of a field-induced phase transition. This second-order transition takes place at a critical field $H_c$ above which the magnetization process is accompanied by a canting of the magnetic moments off their local easy-planes. The specific heat curves for $Hparallel [100]$ ($Hgg H_c$) are well described by a model presuming a single dispersionless excitation mode with the energy gap obtained from the spectroscopic measurements.
The search for quantum spin liquids (QSL) -- topological magnets with fractionalized excitations -- has been a central theme in condensed matter and materials physics. While theories are no longer in short supply, tracking down materials has turned out to be remarkably tricky, in large part because of the difficulty to diagnose experimentally a state with only topological, rather than conventional, forms of order. Pyrochlore systems have proven particularly promising, hosting a classical Coulomb phase in the spin ices Dy/Ho$_2$Ti$_2$O$_7$, with subsequent proposals of candidate QSLs in other pyrochlores. Connecting experiment with detailed theory exhibiting a robust QSL has remained a central challenge. Here, focusing on the strongly spin-orbit coupled effective $S=1/2$ pyrochlore Ce$_2$Zr$_2$O$_7$, we analyse recent thermodynamic and neutron scattering experiments, to identify a microscopic effective Hamiltonian through a combination of finite temperature Lanczos, Monte Carlo and analytical spin dynamics calculations. Its parameter values suggest a previously unobserved exotic phase, a $pi$-flux U(1) QSL. Intriguingly, the octupolar nature of the moments makes them less prone to be affected by crystal imperfections or magnetic impurities, while also hiding some otherwise characteristic signatures from neutrons, making this QSL arguably more stable than its more conventional counterparts.
The gadolinium pyrochlores, Gd$_2B_2$O$_7$, are amongst the best realizations of antiferromagnetically coupled Heisenberg spins on a pyrochlore lattice. We present a magnetic characterization of Gd$_2$Pt$_2$O$_7$, a unique member of this family. Magnetic susceptibility, heat capacity, and muon spin relaxation measurements show that Gd$_2$Pt$_2$O$_7$ undergoes an antiferromagnetic ordering transition at $T_N = 1.6$ K. This transition is strongly first order, as indicated by the sharpness of the heat capacity anomaly, thermal hysteresis in the magnetic susceptibility, and a non-divergent relaxation rate in $mu$SR. The form of the heat capacity below $T_N$ suggests that the ground state is an anisotropic collinear antiferromagnet with an excitation spectrum that is gapped by 0.245(1) meV. The ordering temperature in Gd$_2$Pt$_2$O$_7$, $T_N = 1.6$ K, is a substantial 160% increase from other gadolinium pyrochlores, which have been found to order at 1 K or lower. We attribute this enhancement in $T_N$ to the $B$-site cation, platinum, which, despite being non-magnetic, has a filled $5d$ $t_{2g}$ orbital and an empty $5d$ $e_g$ orbital that can facilitate superexchange. Thus, the magnetic frustration in Gd$_2$Pt$_2$O$_7$ is partially relieved, thereby promoting magnetic order.
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