Long-range order at low temperatures in dipolar spin ice

It has recently been suggested that long-range magnetic dipolar interactions are responsible for spin ice behavior in the Ising pyrochlore magnets Dy2Ti2O7 and Ho2Ti2O7. We report here numerical results on the low temperature properties of the dipolar spin ice model, obtained via a new loop algorithm which greatly improves the dynamics at low temperature. We recover the previously reported missing entropy in this model, and find a first order transition to a long-range ordered phase with zero total magnetization at very low temperature. We discuss the relevance of these results to Dy2Ti2O7 and Ho2Ti2O7.     

Field-induced transition on a triangular plane in the spin-ice compound Dy2Ti2O7

The origin of the lowest-temperature anomaly reported several years ago using a polycrystalline sample of the spin-ice compound Dy2Ti2O7 has remained unresolved. Here we finally clarify its origin by susceptibility measurements down to 65 mK using single crystals under accurate control of the magnetic fields in two independent directions. We demonstrate that the transition is induced under a subtle field combination that precisely cancels the nearest-neighbor spin interactions acting on the spins on the triangular lattice within the pyrochlore structure. Contrary to the other two field-induced transitions, this transition is driven only by the interactions beyond the nearest neighbors. Our observation thus provides the first qualitative evidence for the essential importance of the dipolar interaction beyond the nearest neighbors in the spin ice.     

Kagomé ice state in the dipolar spin ice Dy2Ti2O7

We have investigated the kagomé ice behavior of the dipolar spin-ice compound Dy2Ti2O7 in a magnetic field along a [111] direction using neutron scattering and Monte Carlo simulations. The spin correlations show that the kagomé ice behavior predicted for the nearest-neighbor interacting model, where the field induces dimensional reduction and spins are frustrated in each two-dimensional kagomé lattice, occurs in the dipole interacting system. The spins freeze at low temperatures within the macroscopically degenerate ground states of the nearest-neighbor model.     

Finite-temperature transitions in dipolar spin ice in a large magnetic field

We use Monte Carlo simulations to identify the mechanism that allows for phase transitions in dipolar spin ice to occur and survive for an applied magnetic field H much larger in strength than that of the spin-spin interactions. In the most generic and highest symmetry case, the spins on one out of four sublattices of the pyrochlore decouple from the total local exchange+dipolar+applied field. In the special case where H is aligned perfectly along the [110] crystallographic direction, spin chains perpendicular to H show a transition to q=X long-range order, which proceeds via a one- to three-dimensional crossover. We propose that these transitions are relevant to the origin of specific heat features observed in powder samples of the Dy2Ti2O7 spin ice material for H above 1 Tesla.     

Multiple field-induced phase transitions in the geometrically frustrated dipolar magnet: Gd(2) Ti(2)O(7)

Field-driven phase transitions generally arise from competition between Zeeman energy and exchange or crystal-field anisotropy. Here we present the phase diagram of a frustrated pyrochlore magnet Gd(2)Ti(2)O(7), where crystal-field splitting is small compared to the dipolar energy. We find good agreement between zero-temperature critical fields and those obtained from a mean-field model. Here, dipolar interactions couple real space and spin space, so the transitions in Gd(2)Ti(2)O(7) arise from field-induced "cooperative anisotropy," reflecting the broken spatial symmetries of the pyrochlore lattice.     

Dy2Ti2O7 spin ice: a test case for emergent clusters in a frustrated magnet

Dy2Ti2O7 is a geometrically frustrated magnetic material with a strongly correlated spin ice regime that extends from 1 K down to as low as 60 mK. The diffuse elastic neutron scattering intensities in the spin ice regime can be remarkably well described by a phenomenological model of weakly interacting hexagonal spin clusters, as invoked in other geometrically frustrated magnets. We present a highly refined microscopic theory of Dy2Ti2O7 that includes long-range dipolar and exchange interactions to third nearest neighbors and which demonstrates that the clusters are purely fictitious in this material. The seeming emergence of composite spin clusters and their associated scattering pattern is instead an indicator of fine-tuning of ancillary correlations within a strongly correlated state.     

Unconventional magnetization processes and thermal runaway in spin-ice Dy2Ti2O7

We investigate the nonequilibrium behavior of the spin-ice Dy2Ti2O7 by studying its magnetization as a function of the field sweep rate. Below the enigmatic 'freezing' temperature T(equil)≈600 mK, we find that even the slowest sweeps fail to yield the equilibrium magnetization curve and instead give an initially much flatter curve. For higher sweep rates, the magnetization develops sharp steps accompanied by similarly sharp peaks in the temperature of the sample. We ascribe the former behavior to the energy barriers encountered in the magnetization process, which proceeds via flipping of spins on filaments traced out by the field-driven motion of the gapped, long-range interacting magnetic monopole excitations. The peaks in temperature result from the released Zeeman energy not being carried away efficiently; the resulting heating triggers a chain reaction.     

自旋冰材料R2Ti2O7（R=Dy，Ho）的单晶生长和低温物性研究

本文首先对R2Ti2O7（R=Dy,Ho）单晶的生长条件进行了探索,经过多次尝试,得到了较理想的生长条件,并获得了高品质的单晶．磁化率和比热测量证实了这些单晶材料具有自旋冰基态．另外,通过对不同条件下退火的Dy2Ti2O7单晶低温热传导的深入研究,发现R2Ti2O7单晶具有较小的声子峰,并且退火条件的变化对峰值的影响很...     

Slow spin relaxation in a highly polarized cooperative paramagnet

We report measurements of the ac susceptibility of the cooperative paramagnet Tb2Ti2O7 in a strong magnetic field. Our data show the expected saturation maximum in chi(T) and also an unexpected frequency dependence of this peak at low frequencies (<1 Hz), suggesting very slow spin relaxations are occurring. Measurements on samples diluted with nonmagnetic Y3+ or Lu3+ and complementary measurements on pure and diluted Dy2Ti2O7 strongly suggest that the relaxation is associated with dipolar spin correlations, representing unusual cooperative behavior in a paramagnetic system.     

Microcanonical relation between continuous and discrete spin models

A relation between a class of stationary points of the energy landscape of continuous spin models on a lattice and the configurations of an Ising model defined on the same lattice suggests an approximate expression for the microcanonical density of states. Based on this approximation we conjecture that if a O(n) model with ferromagnetic interactions on a lattice has a phase transition, its critical energy density is equal to that of the n=1 case, i.e., an Ising system with the same interactions. The conjecture holds true in the case of long-range interactions. For nearest-neighbor interactions, numerical results are consistent with the conjecture for n=2 and n=3 in three dimensions. For n=2 in two dimensions (XY model) the conjecture yields a prediction for the critical energy of the Bere?inskij-Kosterlitz-Thouless transition, which would be equal to that of the two-dimensional Ising model. We discuss available numerical data in this respect.     

Evidence for gapped spin-wave excitations in the frustrated Gd2Sn2O7 pyrochlore antiferromagnet from low-temperature specific heat measurements

We have measured the low-temperature specific heat of the geometrically frustrated pyrochlore Heisenberg antiferromagnet Gd2Sn2O7 in zero magnetic field. The specific heat is found to drop exponentially below approximately 350 mK. This provides evidence for a gapped spin-wave spectrum due to an anisotropy resulting from single-ion effects and long-range dipolar interactions. The data are well fitted by linear spin-wave theory, ruling out unconventional low-energy magnetic excitations in this system, and allowing a determination of the pertinent exchange interactions in this material.     

Three-dimensional Kasteleyn transition: spin ice in a [100] field

We examine the statistical mechanics of spin-ice materials with a [100] magnetic field. We show that the approach to saturated magnetization is, in the low-temperature limit, an example of a 3D Kasteleyn transition, which is topological in the sense that magnetization is changed only by excitations that span the entire system. We study the transition analytically and using a Monte Carlo cluster algorithm, and compare our results with recent data from experiments on Dy2Ti2O7.     

Nucleation and metastability in three-dimensional Ising models

We present Monte Carlo experiments on nucleation theory in the nearest-neighbor three-dimensional Ising model and in Ising models with long-range interactions. For the nearest-neighbor model, our results are compatible with the classical nucleation theory (CNT) for low temperatures, while for the long-range model a breakdown of the CNT was observed near the mean-field spinodal. A new droplet model and a zeroth-order theory of droplet growth are also presented.Supported in part by grants from ARO, ONR, and NSF.     

Optimized energy calculation in lattice systems with long-range interactions

We discuss an efficient approach to the calculation of the internal energy in numerical simulations of spin systems with long-range interactions. Although, since the introduction of the Luijten-Blote algorithm, Monte Carlo simulations of these systems no longer pose a fundamental problem, the energy calculation is still an O(N2) problem for systems of size N. We show how this can be reduced to an O(N log N) problem, with a break-even point that is already reached for very small systems. This allows the study of a variety of, until now hardly accessible, physical aspects of these systems. In particular, we combine the optimized energy calculation with histogram interpolation methods to investigate the specific heat of the Ising model and the first-order regime of the three-state Potts model with long-range interactions.     

Why spin ice obeys the ice rules

The low-temperature entropy of the spin ice compounds, such as and , is well described by the nearest-neighbor antiferromagnetic Ising model on the pyrochlore lattice, i.e., by the "ice rules." This is surprising since the dominant coupling between the spins is their long ranged dipole interaction. We show that this phenomenon can be understood rather elegantly: one can construct a model dipole interaction, by adding terms of shorter range, which yields precisely the same ground states, and hence entropy, as the nearest-neighbor interaction. A treatment of the small difference between the model and true dipole interactions reproduces the numerical work by Gingras et al. in detail. We are also led to a more general concept of projective equivalence between interactions.     

Spin waves and quantum criticality in the frustrated XY pyrochlore antiferromagnet Er2Ti2O7

We report detailed measurements of the low temperature magnetic phase diagram of Er2Ti2O7. Heat capacity and time-of-flight neutron scattering studies of single crystals reveal unconventional low-energy states. Er3+ magnetic ions reside on a pyrochlore lattice in Er2Ti2O7, where local XY anisotropy and antiferromagnetic interactions give rise to a unique frustrated system. In zero field, the ground state exhibits coexisting short and long-range order, accompanied by soft collective spin excitations previously believed to be absent. The application of finite magnetic fields tunes the ground state continuously through a landscape of noncollinear phases, divided by a zero temperature phase transition at micro{0}H{c} approximately 1.5 T. The characteristic energy scale for spin fluctuations is seen to vanish at the critical point, as expected for a second order quantum phase transition driven by quantum fluctuations.     

Magnetic ordering in the spin-ice candidate Ho2Ru2O7

Neutron scattering measurements on the spin-ice candidate material Ho2Ru2O7 have revealed two magnetic transitions at T approximately 95 and approximately 1.4 K to long-range ordered states involving the Ru and Ho sublattices, respectively. Between these transitions, the Ho3+ moments form short-ranged ordered spin clusters. The internal field provided by the ordered S=1 Ru4+ moments disrupts the fragile spin-ice state and drives the Ho3+ moments to order. We have directly measured a slight shift in the Ho3+ crystal field levels at 95 K from the Ru ordering.     

Observation of a liquid-gas-type transition in the pyrochlore spin ice compound Dy2Ti2O7 in a magnetic field

Low temperature magnetization measurements on the pyrochlore spin ice compound Dy2Ti2O7 reveal that the ice-rule breaking spin flip, appearing at H approximately 0.9 T applied parallel to the [111] direction, turns into a novel first-order transition for T<0.36 K which is most probably of a liquid-gas type. T-linear variation of the critical field observed down to 0.03 K suggests the unusual situation that the entropy release across the transition remains finite [approximately 0.5 (J/K) x mol-Dy] as T-->0, in accordance with a breaking of the macroscopic degeneracy in the intermediate "kagomé ice" state.     

Phase stability and pressure dependence of defect formation in Gd2Ti2O7 and Gd2Zr2O7 pyrochlores

We report dramatically different behaviors between isostructural Gd2Ti2O7 and Gd2Zr2O7 pyrochlore at pressures up to 44 GPa, in which the substitution of Ti for Zr significantly increases structural stability. Upon release of pressure, the Gd2Ti2O7 becomes amorphous. In contrast, the high-pressure phase of Gd2Zr2O7 transforms to a disordered defect-fluorite structure. First-principle calculations for both compositions revealed that the response of pyrochlore to high pressure is controlled by the intrinsic energetics of defect formation.