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∼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 [∼0.5   (J/K)⋅mol−Dy] as T→0, in accordance with a breaking of the macroscopic degeneracy in the intermediate “kagomé ice” state

Theory of Metal-Insulator Transition in PrRu4P12 and PrFe4P12

All symmetry allowed couplings between the 4f^2-electron ground state doublet of trivalent praseodymium in PrRu4P12 and PrFe4P12 and displacements of the phosphorus, iron or ruthenium ions are considered. Two types of displacements can change the crystal lattice from body-centred cubic to simple orthorhombic or to simple cubic. The first type lowers the point group symmetry from tetrahedral to orthorhombic, while the second type leaves it unchanged, with corresponding space group reductions Im3 --> Pmmm and Im3 --> Pm3 respectively. In former case, the lower point-group symmetry splits the degeneracy of the 4f^2 doublet into states with opposite quadrupole moment, which then leads to anti-quadrupolar ordering, as in PrFe4P12. Either kind of displacement may conspire with nesting of the Fermi surface to cause the metal-insulator or partial metal-insulator transition observed in PrFe4P12 and PrRu4P12. We investigate this scenario using band-structure calculations, and it is found that displacements of the phosphorus ions in PrRu4P12 (with space group reduction Im3 --> Pm3) open a gap everywhere on the Fermi surface.Comment: 6 page

Quantum-Classical Reentrant Relaxation Crossover in Dy2Ti2O7 Spin-Ice

We have studied spin relaxation in the spin ice compound Dy2Ti2O7 through measurements of the a.c. magnetic susceptibility. While the characteristic spin relaxation time is thermally activated at high temperatures, it becomes almost temperature independent below Tcross ~ 13 K, suggesting that quantum tunneling dominates the relaxation process below that temperature. As the low-entropy spin ice state develops below Tice ~ 4 K, the spin relaxation time increases sharply with decreasing temperature, suggesting the emergence of a collective degree of freedom for which thermal relaxation processes again become important as the spins become highly correlated

Metal-insulator transition in PrRu4_4P12_{12} and SmRu4_4P12_{12} investigated by optical spectroscopy

Electronic structures of the filled-skutterudite compounds PrRu$_4$P$_{12}$ and SmRu$_4$P$_{12}$, which undergo a metal-insulator transition (MIT) at $T_{\rm MI}$ = 60 K and 16 K, respectively, have been studied by means of optical spectroscopy. Their optical conductivity spectra develop an energy gap of $\sim$ 10 meV below $T_{\rm MI}$. The observed characteristics of the energy gap are qualitatively different from those of the Kondo semiconductors. In addition, optical phonon peaks in the spectra show anomalies upon the MIT, including broadening and shifts at $T_{\rm MI}$ and an appearance of new peaks below $T_{\rm MI}$. These results are discussed in terms of density waves or orbital ordering previously predicted for these compounds.Comment: 4pages, 4figures, submitted to Physical Review

Dynamic behavior of magnetic avalanches in the spin-ice compound Dy2_2Ti2_2O7_7

Avalanches of the magnetization, that is to say an abrupt reversal of the magnetization at a given field, have been previously reported in the spin-ice compound Dy$_{2}$Ti$_{2}$O$_{7}$. This out-of-equilibrium process, induced by magneto-thermal heating, is quite usual in low temperature magnetization studies. A key point is to determine the physical origin of the avalanche process. In particular, in spin-ice compounds, the origin of the avalanches might be related to the monopole physics inherent to the system. We have performed a detailed study of the avalanche phenomena in three single crystals, with the field oriented along the [111] direction, perpendicular to [111] and along the [100] directions. We have measured the changing magnetization during the avalanches and conclude that avalanches in spin ice are quite slow compared to the avalanches reported in other systems such as molecular magnets. Our measurements show that the avalanches trigger after a delay of about 500 ms and that the reversal of the magnetization then occurs in a few hundreds of milliseconds. These features suggest an unusual propagation of the reversal, which might be due to the monopole motion. The avalanche fields seem to be reproducible in a given direction for different samples, but they strongly depend on the initial state of magnetization and on how the initial state was achieved.Comment: 11 pages, 14 figure

31P-NMR and muSR Studies of Filled Skutterudite Compound SmFe4P12: Evidence for Heavy Fermion Behavior with Ferromagnetic Ground State

The 31P-NMR (nuclear magnetic resonance) and muSR (muon spin relaxation) measurements on the filled skutterudite system SmFe4P12 have been carried out. The temperature T dependence of the 31P-NMR spectra indicates the existence of the crystalline electric field effect splitting of the Sm3+$ (J = 5/2) multiplet into a ground state and an excited state of about 70 K. The spin-lattice relaxation rate 1/T1 shows the typical behavior of the Kondo system, i.e., 1/T1 is nearly T independent above 30 K, and varies in proportion to T (the Korringa behavior, 1/T1 \propto T) between 7.5 K and 30 K. The T dependence deviated from the Korringa behavior below 7 K, which is independent of T in the applied magnetic field of 1 kOe, and suppressed strongly in higher fields. The behavior is explained as 1/T1is determined by ferromagnetic fluctuations of the uncovered Sm3+ magnetic moments by conduction electrons. The muSR measurements in zero field show the appearance of a static internal field associated with the ferromagnetic order below 1.6 K.Comment: 6 pages, 9 figures, to be published in J. Phys. Soc. Jpn. 75 (2006

Dilution effects in Ho2−x_{2-x}Yx_xSn2_2O7_7: from the Spin Ice to the single-ion magnet

A study of the modifications of the magnetic properties of Ho$_{2-x}$Y$_x$Sn$_2$O$_7$ upon varying the concentration of diamagnetic Y$^{3+}$ ions is presented. Magnetization and specific heat measurements show that the Spin Ice ground-state is only weakly affected by doping for $x\leq 0.3$, even if non-negligible changes in the crystal field at Ho$^{3+}$ occur. In this low doping range $\mu$SR relaxation measurements evidence a modification in the low-temperature dynamics with respect to the one observed in the pure Spin Ice. For $x\to 2$, or at high temperature, the dynamics involve fluctuations among Ho$^{3+}$ crystal field levels which give rise to a characteristic peak in $^{119}$Sn nuclear spin-lattice relaxation rate. In this doping limit also the changes in Ho$^{3+}$ magnetic moment suggest a variation of the crystal field parameters.Comment: 4 pages, 5 figures, proceedings of HFM2008 Conferenc

Low Temperature Specific Heat of Dy2_2Ti2_2O7_7 in the Kagome Ice State

We report the specific heat of single crystals of the spin ice compound Dy$_2$Ti$_2$O$_7$ at temperatures down to 100 mK in the so-called Kagome ice state. In our previous paper, we showed the anisotropic release of residual entropy in different magnetic field directions and reported new residual entropy associated with spin frustration in the Kagome slab for field in the [111] direction. In this paper, we confirm the first-order phase transition line in the field-temperature phase diagram and the presence of a critical point at (0.98 T, 400 mK), previously reported from the magnetization and specific-heat data. We newly found another peak in the specific heat at 1.25 T below 0.3 K. One possible explanation for the state between 1 T and 1.25 T is the coexistence of states with different spin configurations including the 2-in 2-out one (Kagome ice state), the 1-in 3-out state (ordered state) and paramagnetic one (free-spin state).Comment: 14 pages, 7 figure

Spin Dynamics at Very Low Temperature in Spin Ice Dy2_2Ti2_2O7_7

We have performed AC susceptibility and DC magnetic relaxation measurements on the spin ice system Dy$_2$Ti$_2$O$_7$ down to 0.08 K. The relaxation time of the magnetization has been estimated below 2 K down to 0.08 K. The spin dynamics of Dy$_2$Ti$_2$O$_7$ is well described by using two relaxation times ($\tau_{\rm S}$ (short time) and $\tau_{\rm L}$ (long time)). Both $\tau_{\rm S}$ and $\tau_{\rm L}$ increase on cooling. Assuming the Arrhenius law in the temperature range 0.5-1 K, we obtained an energy barrier of 9 K. Below 0.5 K, both $\tau_{\rm S}$ and $\tau_{\rm L}$ show a clear deviation from the thermal activated dynamics toward temperature independent relaxation, suggesting a quantum dynamics.Comment: 4 page

Anisotropic Release of the Residual Zero-point Entropy in the Spin Ice Compound Dy2Ti2O7: Kagome-ice Behavior

We report the specific heat and entropy of single crystals of the spin ice compound Dy2Ti2O7 at temperatures down to 0.35 K. We apply magnetic fields along the four characteristic directions: [100], [110], [111] and [112]. Because of Ising anisotropy, we observe anisotropic release of the residual zero-point entropy, attributable to the difference in frustration dimensionality. In the high magnetic field along these four directions, the residual entropy is almost fully released and the activation entropy reaches Rln2. However, in the intermediate field region, the entropy in fields along the [111] direction is different from those for the other three field directions. For the [111] direction the frustration structure changes from that of three-dimensional(3D) pyrochlore to that of two-dimensional(2D) Kagome-like lattice with constraint due to the ice rule, leading to different values of zero-point entropy.Comment: 4 pages, 4 figures, to appear in Phys. Rev.