强耦合磁失措自旋冰系统Dy2Ti2O7单晶生长和基本磁性质测量

利用红外光源浮区法生长出大尺寸、高质量的磁失措自旋冰化合物Dy2Ti2O7单晶体.X射线衍射实验证实晶体具有面心立方结构,空间群为 Fd3m,晶胞参数a＝1.0112(2) nm,[111]和[400]方向X射线衍射摇摆曲线半高宽分别仅为0.07°和0.05°.直流磁化率与温度关系测量给出晶体的Van Vleck顺磁因子为2.46×10-5 m3/mol,有效磁矩μeff＝10.24(4)μB,Cure-Weiss温度ΘCW＝1.1 K,揭示Dy2Ti2O7具有弱的铁磁性.对磁性起源的综合分析表明,该自旋冰晶体磁性质主要来源于磁偶极相互作用,且相关最近邻长程偶极相互作用能量标度Dnn＝3.00 K.     

Temperature‐dependent Raman scattering studies of the geometrically frustrated pyrochlores Dy2Ti2O7, Gd2Ti2O7 and Er2Ti2O7

The temperature‐dependent Raman studies of A₂Ti₂O₇(A = Dy, Er, Gd) were performed on single crystals and polycrystalline samples in the 4.2–295 K temperature range. The Raman spectra showed softening of the majority of phonon modes upon cooling in the whole temperature range studied and large decrease of linewidths. These changes have been analyzed in terms of strong third‐order phonon–phonon anharmonic interactions. Moreover, the 312 and 330 cm⁻¹ modes of Er₂Ti₂O₇(Gd₂Ti₂O₇) showed hardening upon cooling down to about 130 K (100 K) and then anomalous softening below this temperature. The observed anomalous behavior of the Raman modes indicates that some important changes occur in these materials at low temperatures. However, the origin of this behavior is still not clear. Copyright © 2008 John Wiley & Sons, Ltd.     

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.     

First-order transition in the spin dynamics of geometrically frustrated Yb2Ti2O7

Using neutron diffraction, 170Yb M?ssbauer and muon spin relaxation spectroscopies, we have examined the pyrochlore Yb2Ti2O7, where the Yb3+S' = 1/2 ground state has planar anisotropy. Below approximately 0.24 K, the temperature of the known specific-heat lambda transition, there is no long range magnetic order. We show that the transition corresponds to a first-order change in the fluctuation rate of the Yb3+ spins. Above the transition temperature, the rate, in the GHz range, follows a thermal excitation law, whereas below, the rate, in the MHz range, is temperature independent, indicative of a quantum fluctuation regime.     

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.     

Microscopic study of a pressure-induced ferromagnetic-spin-glass transition in the geometrically frustrated pyrochlore (Tb1-xLax)2Mo2O7

We have studied (Tb1-xLax)2Mo2O7 pyrochlores by neutron diffraction and muSR at ambient and under applied pressure. (Tb,La) substitution expands the lattice and induces a change from a spin-glass-like state (x=0) to a noncollinear ferromagnet (x=0.2). In the ferromagnetic structure, the Tb moments orient close to their local anisotropy axes as for an ordered spin ice, while the Mo ones orient close to the net moment. The temperature dependence of the muSR relaxation rates and static local fields suggests a second transition of dynamical nature below the Curie transition. Under pressure, the long range order breaks down and a spin-glass-like state is recovered. The whole set of data provides a microscopic picture of the spin correlations and fluctuations in the region of the ferromagnetic-spin-glass threshold.     

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.     

Oxygen ion conductivity in doped Gd2Ti2O7 with the pyrochlore structure

Materials with the A₂B₂O₇ pyrochlore structure have interesting ionic transport properties because of their crystallographic structure, which can be described as a stable array of corner-shared BO₆ octahedra that is penetrated by a 3-dimensional tunnel configuration that is partly filled by the A₂O sublattice. The pyrochlore stochiometry means that there are built-in intrinsic oxide ion vacancies in the crystal structure in comparison to the related fluorite type structure. These are in the A₂O sublattice, so that the tunnels are only 75% occupied. The presence of these tunnels leads to the possibility of significant changes in the composition, and some ionic species in this sublattice exhibit high mobility. The cubic pyrochlore Gd₂Ti₂O₇ was doped in various ways to change its ionic and electronic transport properties. The total conductivity and partial ionic and electronic contributions were investigated by ac impedance and EMF measurement techniques. The influence of either A or B site doping with aliovalent ions that occupy sites in the A₂O and B₂O₆ sublattices was investigated. The results of these experiments are presented and discussed in relation to the crystal structure and defect chemistry of this family of oxides. Paper presented at the 2nd Euroconference on Solid State Ionics, Funchal, Madeira, Portugal, Sept. 10–16, 1995     

Experimental observations of ferroelectricity in double pyrochlore Dy2Ru2O7

Double pyrochlore Dy2Ru207 is synthesized and its magnetism and ferroelectricity below the Ru4＋ spin ordering temperature （NI00 K） are investigated. The ferroelectric transition appears at -18 K, much higher than the Dy3＋ spin ordering point at -1.8 K and lower than the Ru4＋ spin ordering point at -100 K. The measured electric polarization at ,-2 K is as big as 145℃/m2 in the polycrystalline samples. It is argued that the ferroelectricity is possibly ascribed to the electric dipole ordering arising from the collective monopole excitations in the Dy3＋ tetrahedrons in prior to the Dy3＋ spin ordering into spin-ice like state below -1.8 K.     

Spontaneous formation of vanadium "molecules" in a geometrically frustrated crystal: AlV2O4

We investigated the charge-ordered (CO) state in spinel AlV2O4 by electron diffraction, synchrotron x-ray diffraction, and magnetic measurements. It was found that the CO structure appearing below 700 K is characterized by the formation of V clusters (heptamers), each of which is consisting of 7 vanadium atoms and is in a spin-singlet state as a total. Theoretical consideration indicates that this unique molecularlike V heptamer is stabilized by a strong bonding of vanadium t(2g) orbitals.     

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.     

Quadrupole interactions and relaxation effects in Dy2Ti2O7

Studies of quadrupole interactions and relaxation phenomena in Dy₂Ti₂O₇ at various temperatures up to 750 K have been performed using the Mössbauer effect of the 25.6 keV transition in ¹⁶¹Dy. The source used was ¹⁶¹Tb in ¹⁶⁰Gd₂Ti₂O₇ at 150 K, which emits a very narrow 25.6 keV γ line. Quadrupole interaction parameters and relaxation times, as function of temperature, were deduced from the measurements.     

Quantum-classical reentrant relaxation crossover in Dy2Ti2O7 spin ice

We have studied spin relaxation in the spin ice compound Dy2Ti2O7 through measurements of the ac magnetic susceptibility. While the characteristic spin-relaxation time (tau) is thermally activated at high temperatures, it becomes almost temperature independent below T(cross) approximately 13 K. This behavior, combined with nonmonotonic magnetic field dependence of tau, indicates that quantum tunneling dominates the relaxational process below that temperature. As the low-entropy spin ice state develops below T(ice) approximately 4 K, tau 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 strongly correlated.     

Phase diagram of a geometrically frustrated triangular-lattice antiferromagnet in a magnetic field

The magnetic phase diagram of a geometrically frustrated triangular-lattice antiferromagnet is evaluated as a function of magnetic field and anisotropy using a trial spin state built from harmonics of a fundamental ordering wave vector. A noncollinear incommensurate state, observed to be chiral and ferroelectric in CuFeO2, appears above a collinear state with 4 sublattices (SLs). The apparent absence of multiferroic behavior for predicted chiral, noncollinear 5-SL states poses a challenge to theories of the ferroelectric coupling in CuFeO2.     

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.     

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.     

Pressure and field induced magnetic order in the spin liquid Tb2Ti2O7 as studied by single crystal neutron diffraction

We have studied the spin liquid Tb2Ti2O7 by single crystal neutron diffraction under high pressure up to 2.8 GPa, together with uniaxial stress, down to 0.1 K, in zero and high magnetic fields up to 7 T. In zero magnetic field, a long-range ordered antiferromagnetic structure is induced by pressure. The Néel temperature and ordered magnetic moment can be tuned by the anisotropic pressure component. Under magnetic field, the antiferromagnetic structure transforms into a canted ferromagnetic one at 0.6 T. Spin canting persists even at 7 T. The magnetic phase diagram under pressure shows a strong increase of the Néel temperature with the field.     

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.