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Register a new userAbsence of long-range order in an $XY$ pyrochlore antiferromagnet Er$_2$AlSbO$_7$
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Rare-earth pyrochlores are known to exhibit exotic magnetic phenomena. We report a study of crystal growth and characterizations of a new rare-earth compound Er$_2$AlSbO$_7$, in which Al$^{3+}$ and Sb$^{5+}$ ions share the same positions with a random distribution. The magnetism are studied by magnetic susceptibility, specific heat and thermal conductivity measurements at low temperatures down to several tens of milli-kelvin. Different from the other reported Er-based pyrochlores exhibiting distinct magnetically ordered states, a spin-freezing transition is detected in Er$_2$AlSbO$_7$ below 0.37 K, which is primarily ascribed to the inherent structural disorder. A cluster spin-glass state is proposed in view of the frequency dependence of the peak position in the ac susceptibility. In addition, the temperature and field dependence of thermal conductivity indicates rather strong spin fluctuations which is probably due to the phase competition.
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Er$_2$Sn$_2$O$_7$ remains a puzzling case among the extensively studied frustrated compounds of the rare-earth pyrochlore family. Indeed, while a first order transition towards a long-range antiferromagnetic state with the so-called Palmer-Chalker structure is theoretically predicted, it has not been observed yet, leaving the issue, as to whether it is a spin-liquid candidate, open. We report on neutron scattering and magnetization measurements which evidence a second order transition towards this Palmer-Chalker ordered state around 108 mK. Extreme care was taken to ensure a proper thermalization of the sample, which has proved to be crucial to successfully observe the magnetic Bragg peaks. At the transition, a gap opens in the excitations, superimposed on a strong quasielastic signal. The exchange parameters, refined from a spin wave analysis in applied magnetic field, confirm that Er$_2$Sn$_2$O$_7$ is a realization of the dipolar XY pyrochlore antiferromagnet. The proximity of competing phases and the strong XY anisotropy of the Er$^{3+}$ magnetic moment might be at the origin of enhanced fluctuations, leading to the unexpected nature of the transition, the low ordering temperature, and the observed multi-scale dynamics.
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.
We explore the field-temperature phase diagram of the XY pyrochlore antiferromagnet Er$_2$Ti$_2$O$_7$, by means of magnetization and neutron diffraction experiments. Depending on the field strength and direction relative to the high symmetry cubic directions $[001], [1bar{1}0]$ and $[111]$, the refined field induced magnetic structures are derived from the zero field $psi_2$ and $psi_3$ states of the $Gamma_5$ irreducible representation which describes the ground state of XY pyrochlore antiferromagnets. At low field, domain selection effects are systematically at play. In addition, for $[001]$, a phase transition is reported towards a $psi_3$ structure at a characteristic field $H_c^{001}=$ 43 mT. For $[1bar{1}0]$ and $[111]$, the spins are continuously tilted by the field from the $psi_2$ state, and no phase transition is found while domain selection gives rise to sharp anomalies in the field dependence of the Bragg peaks intensity. For $[1bar{1}0]$, these results are confirmed by high resolution inelastic neutron scattering experiments, which in addition allow us to determine the field dependence of the spin gap. This study agrees qualitatively with the scenario proposed theoretically by Maryasin {it et al.} [Phys. Rev. B {bf 93}, 100406(R) (2016)], yet the strength of the field induced anisotropies is significantly different from theory.
Both amorphous and crystalline materials frequently exhibit low temperature specific heats in excess of what is predicted using the Debye model. The signature of this excess specific heat is a peak observed in $C/T^3$ textit{versus} $T$. To understand the curious absence of long-range ordering of local distortions in the crystal structure of pyrochlore Bi$_2$Ti$_2$O$_7$, we have measured the specific heat of crystalline Bi$_2$Ti$_2$O$_7$ and related compounds. We find that the peak in $C/T^3$ versus $T$ in Bi$_2$Ti$_2$O$_7$ falls at a substantially lower temperature than other similar compounds, consistent with the presence of disorder. This thermodynamic evidence for disorder in crystalline Bi$_2$Ti$_2$O$_7$ is consistent with quenched configurational disorder among Bi lone pairs produced by geometrical frustration, which could represent a possible realization of charge ice.
The XY pyrochlore antiferromagnet Er$_2$Ti$_2$O$_7$ exhibits a rare case of $Z_6$ discrete symmetry breaking in its $psi_2$ magnetic ground state. Despite being well-studied theoretically, systems with high discrete symmetry breakings are uncommon in nature and, thus, Er$_2$Ti$_2$O$_7$ provides an experimental playground for the study of broken $Z_n$ symmetry, for $n>2$. A recent theoretical work examined the effect of a magnetic field on a pyrochlore lattice with broken $Z_6$ symmetry and applied it to Er$_2$Ti$_2$O$_7$. This study predicted multiple domain transitions depending on the crystallographic orientation of the magnetic field, inducing rich and controllable magnetothermodynamic behavior. In this work, we present neutron scattering measurements on Er$_2$Ti$_2$O$_7$ with a magnetic field applied along the [001] and [111] directions, and provide the first experimental observation of these exotic domain transitions. In a [001] field, we observe a $psi_2$ to $psi_3$ transition at a critical field of 0.18$pm$0.05T. We are thus able to extend the concept of the spin-flop transition, which has long been observed in Ising systems, to higher discrete $Z_n$ symmetries. In a [111] field, we observe a series of domain-based phase transitions for fields of 0.15$pm$0.03T and 0.40$pm$0.03T. We show that these field-induced transitions are consistent with the emergence of two-fold, three-fold and possibly six-fold Zeeman terms. Considering all the possible $psi_2$ and $psi_3$ domains, these Zeeman terms can be mapped onto an analog clock - exemplifying a literal clock anisotropy. Lastly, our quantitative analysis of the [001] domain transition in Er$_2$Ti$_2$O$_7$ is consistent with order-by-disorder as the dominant ground state selection mechanism.
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