Pauling Entropy, Metastability, and Equilibrium in Dy_{2}Ti_{2}O_{7} Spin Ice

Determining the fate of the Pauling entropy in the classical spin ice material Dy_{2}Ti_{2}O_{7} with respect to the third law of thermodynamics has become an important test case for understanding the existence and stability of ice-rule states in general. The standard model of spin ice-the dipolar spin ice model-predicts an ordering transition at T≈0.15  K, but recent experiments by Pomaranski et al. suggest an entropy recovery over long timescales at temperatures as high as 0.5 K, much too high to be compatible with the theory. Using neutron scattering and specific heat measurements at low temperatures and with long timescales (0.35  K/10^{6}  s and 0.5  K/10^{5}  s, respectively) on several isotopically enriched samples, we find no evidence of a reduction of ice-rule correlations or spin entropy. High-resolution simulations of the neutron structure factor show that the spin correlations remain well described by the dipolar spin ice model at all temperatures. Furthermore, by careful consideration of hyperfine contributions, we conclude that the original entropy measurements of Ramirez et al. are, after all, essentially correct: The short-time relaxation method used in that study gives a reasonably accurate estimate of the equilibrium spin ice entropy due to a cancellation of contributions

Pauling Entropy, Metastability, and Equilibrium in Dy_{2}Ti_{2}O_{7} Spin Ice

Determining the fate of the Pauling entropy in the classical spin ice material Dy_{2}Ti_{2}O_{7} with respect to the third law of thermodynamics has become an important test case for understanding the existence and stability of ice-rule states in general. The standard model of spin ice-the dipolar spin ice model-predicts an ordering transition at T≈0.15  K, but recent experiments by Pomaranski et al. suggest an entropy recovery over long timescales at temperatures as high as 0.5 K, much too high to be compatible with the theory. Using neutron scattering and specific heat measurements at low temperatures and with long timescales (0.35  K/10^{6}  s and 0.5  K/10^{5}  s, respectively) on several isotopically enriched samples, we find no evidence of a reduction of ice-rule correlations or spin entropy. High-resolution simulations of the neutron structure factor show that the spin correlations remain well described by the dipolar spin ice model at all temperatures. Furthermore, by careful consideration of hyperfine contributions, we conclude that the original entropy measurements of Ramirez et al. are, after all, essentially correct: The short-time relaxation method used in that study gives a reasonably accurate estimate of the equilibrium spin ice entropy due to a cancellation of contributions

Multiple Coulomb phase in the fluoride pyrochlore CsNiCrF6

The Coulomb phase is an idealized state of matter whose properties are determined by factors beyond conventional considerations of symmetry, including global topology, conservation laws and emergent order. Theoretically, Coulomb phases occur in ice-type systems such as water ice and spin ice; in dimer models; and in certain spin liquids. However, apart from ice-type systems, more general experimental examples are very scarce. Here we study the partly disordered material CsNiCrF6 and show that this material is a multiple Coulomb phase with signature correlations in three degrees of freedom: charge configurations, atom displacements and spin configurations. We use neutron and X-ray scattering to separate these correlations and to determine the magnetic excitation spectrum. Our results show how the structural and magnetic properties of apparently disordered materials may inherit, and be dictated by, a hidden symmetry—the local gauge symmetry of an underlying Coulomb phase

Temperature-induced phase transition from cycloidal to collinear antiferromagnetism in multiferroic Bi0.9Sm0.1FeO3 driven by f-d induced magnetic anisotropy

In multiferroic BiFeO3 a cycloidal antiferromagnetic structure is coupled to a large electric polarization at room temperature, giving rise to magnetoelectric functionality that may be exploited in novel multiferroic-based devices. In this paper, we demonstrate that substituting samarium for 10% of the bismuth ions increases the periodicity of the room-temperature cycloid, and upon cooling to below ∼15 K the magnetic structure tends towards a simple G-type antiferromagnet, which is fully established at 1.5 K. We show that this transition results from f-d exchange coupling, which induces a local anisotropy on the iron magnetic moments that destroys the cycloidal order - a result of general significance regarding the stability of noncollinear magnetic structures in the presence of multiple magnetic sublattices

Quasiparticle Breakdown and Spin Hamiltonian of the Frustrated Quantum Pyrochlore Yb2Ti2O7Yb_{2}Ti_{2}O_{7} in a Magnetic Field

The frustrated pyrochlore magnet $Yb_{2}Ti_{2}O_{7}$ has the remarkable property that it orders magnetically but has no propagating magnons over wide regions of the Brillouin zone. Here we use inelastic neutron scattering to follow how the spectrum evolves in cubic-axis magnetic fields. At high fields we observe, in addition to dispersive magnons, a two-magnon continuum, which grows in intensity upon reducing the field and overlaps with the one-magnon states at intermediate fields leading to strong renormalization of the dispersion relations, and magnon decays. Using heat capacity measurements we find that the low- and high-field regions are smoothly connected with no sharp phase transition, with the spin gap increasing monotonically in field. Through fits to an extensive data set of dispersion relations combined with magnetization measurements, we reevaluate the spin Hamiltonian, finding dominant quantum exchange terms, which we propose are responsible for the anomalously strong fluctuations and quasiparticle breakdown effects observed at low fields

Temperature-induced phase transition from cycloidal to collinear antiferromagnetism in multiferroic Bi0.9Sm0.1FeO3 driven by f-d induced magnetic anisotropy

In multiferroic BiFeO3 a cycloidal antiferromagnetic structure is coupled to a large electric polarization at room temperature, giving rise to magnetoelectric functionality that may be exploited in novel multiferroic-based devices. In this paper, we demonstrate that substituting samarium for 10% of the bismuth ions increases the periodicity of the room-temperature cycloid, and upon cooling to below ∼15 K the magnetic structure tends towards a simple G-type antiferromagnet, which is fully established at 1.5 K. We show that this transition results from f-d exchange coupling, which induces a local anisotropy on the iron magnetic moments that destroys the cycloidal order - a result of general significance regarding the stability of noncollinear magnetic structures in the presence of multiple magnetic sublattices