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Anomalously slow spin dynamics and short-range correlations in the quantum spin ice systems Yb2Ti2O7 and Yb2Sn2O7

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 Publication date 2015
  fields Physics
and research's language is English




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We report a positive muon spin relaxation and rotation (muSR) study of the quantum spin ice materials Yb2Ti2O7 and Yb2Sn2O7 focusing on the low field response. In agreement with earlier reports, data recorded in small longitudinal fields evidence anomalously slow spin dynamics in the microsecond range below the temperature T_c at which the specific heat displays an intense peak, namely T_c = 0.24 K and 0.15 K, respectively, for the two systems. We found that slow dynamics extends above T_c up to at least 0.7 K for both compounds. The conventional dynamical Gaussian Kubo-Toyabe model describes the muSR spectra recorded above T_c. At lower temperatures a published analytical extension of the Gaussian Kubo-Toyabe model provides a good description, consistent with the existence of short-range magnetic correlations. While the physical response of the two systems is qualitatively the same, Yb2Ti2O7 exhibits a much larger local magnetic susceptibility than Yb2Sn2O7 below T_c. Considering previously reported ac susceptibility, neutron scattering and muSR results, we suggest the existence of anomalously slow spin dynamics to be a common physical property of pyrochlore magnetic materials. The possibility of molecular spin substructures to be associated to the slow dynamics and therefore the short-range correlations is mentioned. The slow spin dynamics observed under field does not exclude the presence of much faster dynamics detected in extremely low or zero field.



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We use numerical linked cluster (NLC) expansions to compute the specific heat, C(T), and entropy, S(T), of a quantum spin ice model of Yb2Ti2O7 using anisotropic exchange interactions recently determined from inelastic neutron scattering measurements and find good agreement with experimental calorimetric data. In the perturbative weak quantum regime, this model has a ferrimagnetic ordered ground state, with two peaks in C(T): a Schottky anomaly signalling the paramagnetic to spin ice crossover followed at lower temperature by a sharp peak accompanying a first order phase transition to the ferrimagnetic state. We suggest that the two C(T) features observed in Yb2Ti2O7 are associated with the same physics. Spin excitations in this regime consist of weakly confined spinon-antispinon pairs. We suggest that conventional ground state with exotic quantum dynamics will prove a prevalent characteristic of many real quantum spin ice materials.
144 - J. Robert , E. Lhotel , G. Remenyi 2015
In this work, we show that the zero field excitation spectra in the quantum spin ice candidate pyrochlore compound ybti is a continuum characterized by a very broad and almost flat dynamical response which extends up to $1-1.5$ meV, coexisting or not with a quasi-elastic response depending on the wave-vector. The spectra do not evolve between 50 mK and 2 K, indicating that the spin dynamics is only little affected by the temperature in both the short-range correlated and ordered regimes. Although classical spin dynamics simulations qualitatively capture some of the experimental observations, we show that they fail to reproduce this broad continuum. In particular, the simulations predict an energy scale twice smaller than the experimental observations. This analysis is based on a careful determination of the exchange couplings, able to reproduce both the zero field diffuse scattering and the spin wave spectrum rising in the field polarized state. According to this analysis, ybti lies at the border between a ferro and an antiferromagnetic phase. These results suggest that the unconventional ground state of ybti is governed by strong quantum fluctuations arising from the competition between those phases. The observed spectra may correspond to a continuum of deconfined spinons as expected in quantum spin liquids.
We report on the non-equilibrium monopole dynamics in the classical spin ice Dy$_2$Ti$_2$O$_7$ detected by means of high-resolution magnetostriction measurements. Significant lattice changes occur at the transition from the kagome-ice to the saturated-ice phase, visible in the longitudinal and transverse magnetostriction. A hysteresis opening at temperatures below 0.6 K suggests a first-order transition between the kagome and saturated state. Extremely slow lattice relaxations, triggered by changes of the magnetic field, were observed. These lattice-relaxation effects result from non-equilibrium monopole formation or annihilation processes. The relaxation times extracted from our experiment are in good agreement with theoretical predictions with decay constants of the order of $10{^4}$ s at 0.3 K.
The pyrochlore material Yb2Ti2O7 displays unexpected quasi-two-dimensional (2D) magnetic correlations within a cubic lattice environment at low temperatures, before entering an exotic disordered ground state below T=265mK. We report neutron scattering measurements of the thermal evolution of the 2D spin correlations in space and time. Short range three dimensional (3D) spin correlations develop below 400 mK, accompanied by a suppression in the quasi-elastic (QE) scattering below ~ 0.2 meV. These show a slowly fluctuating ground state with spins correlated over short distances within a kagome-triangular-kagome (KTK) stack along [111], which evolves to isolated kagome spin-stars at higher temperatures. Furthermore, low-temperature specific heat results indicate a sample dependence to the putative transition temperature that is bounded by 265mK, which we discuss in the context of recent mean field theoretical analysis.
We present an experimental study of the quantum spin ice candidate pyrochlore coumpound przr by means of magnetization measurements, specific heat and neutron scattering up to 12 T and down to 60 mK. When the field is applied along the $[111]$ and $[1bar{1}0]$ directions, ${bf k}=0$ field induced structures settle in. We find that the ordered moment rises slowly, even at very low temperature, in agreement with macroscopic magnetization. Interestingly, for $H parallel [1bar{1}0]$, the ordered moment appears on the so called $alpha$ chains only. The spin excitation spectrum is essentially {it inelastic} and consists in a broad flat mode centered at about 0.4 meV with a magnetic structure factor which resembles the spin ice pattern. For $H parallel [1bar{1}0]$ (at least up to 2.5 T), we find that a well defined mode forms from this broad response, whose energy increases with $H$, in the same way as the temperature of the specific heat anomaly. We finally discuss these results in the light of mean field calculations and propose a new interpretation where quadrupolar interactions play a major role, overcoming the magnetic exchange. In this picture, the spin ice pattern appears shifted up to finite energy because of those new interactions. We then propose a range of acceptable parameters for przr, that allow to reproduce several experimental features observed under field. With these parameters, the actual ground state of this material would be an antiferroquadrupolar liquid with spin-ice like excitations.
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