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Register a new userSleuthing out exotic quantum spin liquidity in the pyrochlore magnet Ce$_2$Zr$_2$O$_7$
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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.
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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.
We investigate the temperature dependence of the spin dynamics in the pyrochlore magnet Nd$_2$Zr$_2$O$_7$ by neutron scattering experiments. At low temperature, this material undergoes a transition towards an all in - all out antiferromagnetic phase and the spin dynamics encompass a dispersion-less mode, characterized by a dynamical spin ice structure factor. Unexpectedly, this mode is found to survive above $T_{rm N} approx 300$ mK. Concomitantly, elastic correlations of the spin ice type develop. These are the signatures of a peculiar correlated paramagnetic phase which can be considered as a new example of Coulomb phase. Our observations near $T_{rm N}$ do not reproduce the signatures expected for a Higgs transition, but show reminiscent features of the all in - all out order superimposed on a Coulomb phase.
The Ce$^{3+}$ pseudospin-$frac{1}{2}$ degrees of freedom in the pyrochlore magnet Ce$_2$Zr$_2$O$_7$ are known to possess dipole-octupole (DO) character, making it a candidate for novel quantum spin liquid (QSL) ground states at low temperatures. We report new heat capacity ($C_p$) measurements on Ce$_2$Zr$_2$O$_7$ which rise sharply at low temperatures, initially plateauing near 0.08 K, before falling off towards a high temperature zero beyond 3 K. Above $sim$0.5 K, the $C_p$ data set can be fit to the results of a quantum numerical linked cluster (NLC) calculation, that allows estimates for the terms in the XYZ Hamiltonian expected for such DO pyrochlore systems. Fits of the same theory to the temperature dependence of neutron scattering and magnetic susceptibility complement this analysis to produce robust estimates of the exchange parameters. Polarized neutron diffraction results show spin flip scattering with pinch points, largely consistent with predictions from the NLC calculation. However, the non-spin flip structure factor shows zone-boundary scattering similar to that observed in the dipolar spin ice Ho$_2$Ti$_2$O$_7$ and likely arising from long-range dipolar interactions. We conclude that Ce$_2$Zr$_2$O$_7$ realizes a U(1)$_pi$ QSL state at low temperatures, and one that resides near the boundary between dipolar and octupolar character. We then interpolate between the NLC-calculated $T$ $>$ $sim$0.5 K $C_p$ and a low temperature form for $C_p$ that is consistent with both the calculated near-neighbour exchange parameters and a $T^3$ $C_p$ appropriate for emergent gapless photons. This low temperature form for $C_p$ allows for $Rln(2)$ entropy to be accounted for up to $T$ = 10 K. Phenomenologically, the entropy recovery above the plateau in $C_p$, near $T$ = 0.08 K, gives $Rln(2)$ less $frac{R}{2}ln(frac{3}{2}$), the missing Pauling, spin ice entropy.
By combining neutron scattering and magnetization measurements down to 80 mK, we determine the $(H,T)$ phase diagram of the Nd$_2$(Zr$_{1-x}$Ti$_x$)$_2$O$_7$ pyrochlore magnet compounds. In those samples, Zr is partially substituted by Ti, hence tuning the exchange parameters and testing the robustness of the various phases. In all samples, the ground state remains all in / all out, while the field induces phase transitions towards new states characterized by 2 in - 2 out or 1 out - 3 in / 1 in - 3 out configurations. These transitions manifest as metamagnetic singularities in the magnetization vs field measurements. Strikingly, it is found that moderate substitution reinforces the stability of the all in / all out phase: the Neel temperature, the metamagnetic fields along with the ordered magnetic moment are higher in substituted samples with $x <$ 10%.
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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