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Register a new userSoftening of breathing elastic mode and trigonal elastic mode in disordered pyrochlore magnet NaCaCo$_2$F$_7$
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Cobalt pyrochlore fluoride NaCaCo$_2$F$_7$ is a disordered frustrated magnet composed of Co$^{2+}$ ions with an effective spin-$frac{1}{2}$ magnetic moment and exhibits spin freezing below $T_f sim$2.4 K. We perform ultrasound velocity measurements on a single crystal of the cubic NaCaCo$_2$F$_7$. The temperature dependence of the bulk modulus (the breathing elastic mode) exhibits Curie-type softening upon cooling below $sim$20 K down to $T_f$, which is suppressed by the magnetic field. This Curie-type softening should be a precursor to the enhancement of the strength of exchange disorder via the spin-lattice coupling, which causes the spin freezing. In contrast to the magnetic-field-suppressed Curie-type softening in the bulk modulus, the trigonal shear modulus exhibits softening with a characteristic minimum upon cooling, which is enhanced by the magnetic field at temperatures below $sim$20 K. This magnetic-field-enhanced elastic anomaly in the trigonal shear modulus suggests a coupling of the lattice to the dynamical spin-cluster state. For NaCaCo$_2$F$_7$, the observed elastic anomalies reveal an occurrence of magnetic-field-induced crossover from an isostructural lattice instability toward the spin freezing to a trigonal lattice instability arising from the emergent dynamical spin-cluster state.
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We present time-of-flight neutron total scattering and polarized neutron scattering measurements of the magnetically frustrated compounds NaCaCo$_2$F$_7$ and NaSrCo$_2$F$_7$, which belong to a class of recently discovered pyrochlore compounds based on transition metals and fluorine. The magnetic pair distribution function (mPDF) technique is used to analyze and model the total scattering data in real space. We find that a previously-proposed model of short-range XY-like correlations with a length scale of 10-15 AA, combined with nearest-neighbor collinear antiferromagnetic correlations, accurately describes the mPDF data at low temperature, confirming the magnetic ground state in these materials. This model is further verified by the polarized neutron scattering data. From an analysis of the temperature dependence of the mPDF and polarized neutron scattering data, we find that short-range correlations persist on the nearest-neighbor length scale up to 200 K, approximately two orders of magnitude higher than the spin freezing temperatures of these compounds. These results highlight the opportunity presented by these new pyrochlore compounds to study the effects of geometric frustration at relatively high temperatures, while also advancing the mPDF technique and providing a novel opportunity to investigate a genuinely short-range-ordered magnetic ground state directly in real space.
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.
By means of ac magnetic-susceptibility measurements, we find evidence for a new magnetic phase of Tb$_2$Ti$_2$O$_7$ below about 140 mK in zero magnetic field. In magnetic fields parallel to [111], this phase---exhibiting frequency- and amplitude-dependent susceptibility and an extremely slow spin dynamics---extends to about 70 mT, at which it gives way to another phase. The field dependence of the susceptibility of this second phase, which extends to about 0.6 T, indicates the presence of a weak magnetization plateau below 50 mK, as has been predicted by a single-tetrahedron four-spin model, giving support to the underlying proposal that the disordered low-field ground state of Tb$_2$Ti$_2$O$_7$ is a quantum spin ice.
The single ion physics of Ho$_2$Ti$_2$O$_7$ is well-understood to produce strong Ising anisotropy, which is an essential ingredient to its low-temperature spin ice state. We present inelastic neutron scattering measurements on Ho$_2$Ti$_2$O$_7$ that reveal a clear inconsistency with its established single ion Hamiltonian. Specifically, we show that a crystal field doublet near 60~meV is split by approximately 3~meV. Furthermore, this crystal field splitting is not isolated to Ho$_2$Ti$_2$O$_7$ but can also be found in its chemical pressure analogs, Ho$_2$Ge$_2$O$_7$ and Ho$_2$Sn$_2$O$_7$. We demonstrate that the origin of this effect is a vibronic bound state, resulting from the entanglement of a phonon and crystal field excitation. We derive the microscopic Hamiltonian that describes the magneto-elastic coupling and provides a quantitative description of the inelastic neutron spectra.
Critical phenomenon at the phase transition reveals the universal and long-distance properties of the criticality. We study the ferromagnetic criticality of the pyrochlore magnet Lu$_2$V$_2$O$_7$ at the ferromagnetic transition ${T_text{c}approx 70, text{K}}$ from the isotherms of magnetization $M(H)$ via an iteration process and the Kouvel-Fisher method. The critical exponents associated with the transition are determined as ${beta = 0.32(1)}$, ${gamma = 1.41(1)}$, and ${delta = 5.38}$. The validity of these critical exponents is further verified by scaling all the $M(H)$ data in the vicinity of $T_text{c}$ onto two universal curves in the plot of $M/|varepsilon|^beta$ versus $H/|varepsilon|^{beta+gamma}$, where ${varepsilon = T/T_text{c} -1}$. The obtained $beta$ and $gamma$ values show asymmetric behaviors on the ${T < T_text{c}}$ and the ${T > T_text{c}}$ sides, and are consistent with the predicted values of 3D Ising and cubic universality classes, respectively. This makes Lu$_2$V$_2$O$_7$ a rare example in which the critical behaviors associated with a ferromagnetic transition belong to different universality classes. We describe the observed criticality from the Ginzburg-Landau theory with the quartic cubic anisotropy that microscopically originates from the anti-symmetric Dzyaloshinskii-Moriya interaction as revealed by recent magnon thermal Hall effect and theoretical investigations.
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