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Slow spin tunneling in the paramagnetic phase of the pyrochlore Nd2Sn2O7

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 نشر من قبل P. Dalmas de Reotier
 تاريخ النشر 2017
  مجال البحث فيزياء
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The insulating pyrochlore compound Nd2Sn2O7 has been shown to undergo a second order magnetic phase transition at Tc ~ 0.91 K to a noncoplanar all-in--all-out magnetic structure of the Nd3+ magnetic moments. An anomalously slow paramagnetic spin dynamics has been evidenced from neutron backscattering and muon spin relaxation (muSR). In the case of muSR this has been revealed through the strong effect of a 50 mT longitudinal field on the spin-lattice relaxation rate. Here, motivated by a recent successful work performed for Yb2Ti2O7 and Yb2Sn2O7, analyzing the shape of the muSR longitudinal polarization function, we substantiate the existence of extremely slow paramagnetic spin dynamics in the microsecond time range for Nd2Sn2O7. Between 1.7 and 7 K, this time scale is temperature independent. This suggests a double spin-flip tunneling relaxation mechanism to be at play, probably involving spin substructures such as tetrahedra. Unexpectedly, the standard deviation of the field distribution at the muon site increases as the system is cooled. This exotic spin dynamics is in sharp contrast with the dynamics above 100 K which is driven by the Orbach relaxation mechanism involving single Nd3+ magnetic moments.



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We report measurements performed on a polycrystalline sample of the pyrochlore compound Nd2Sn2O7. It undergoes a second order magnetic phase transition at Tc ~ 0.91 K to a noncoplanar all-in-all-out magnetic structure of the Nd3+ magnetic moments. Th e thermal behavior of the low temperature specific heat fingerprints excitations with linear dispersion in a three-dimensional lattice. The temperature independent spin-lattice relaxation rate measured below Tc and the anomalously slow paramagnetic spin dynamics detected up to ~ 30 Tc are suggested to be due to magnetic short-range correlations in unidimensional spin clusters, i.e., spin loops. The observation of a spontaneous field in muon spin relaxation measurements is associated with the absence of a divergence-free field for the ground state of an all-in-all-out pyrochlore magnet as predicted recently.
Magnetic systems with spins sitting on a lattice of corner sharing regular tetrahedra have been particularly prolific for the discovery of new magnetic states for the last two decades. The pyrochlore compounds have offered the playground for these st udies, while little attention has been comparatively devoted to other compounds where the rare earth R occupies the same sub-lattice, e.g. the spinel chalcogenides CdR2X4 (X = S, Se). Here we report measurements performed on powder samples of this series with R = Yb using specific heat, magnetic susceptibility, neutron diffraction and muon-spin-relaxation measurements. The two compounds are found to be magnetically similar. They long-range order into structures described by the Gamma_5 irreducible representation. The magnitude of the magnetic moment at low temperature is 0.77 (1) and 0.62 (1) mu_B for X = S and Se, respectively. Persistent spin dynamics is present in the ordered states. The spontaneous field at the muon site is anomalously small, suggesting magnetic moment fragmentation. A double spin-flip tunneling relaxation mechanism is suggested in the cooperative paramagnetic state up to 10 K. The magnetic space groups into which magnetic moments of systems of corner-sharing regular tetrahedra order are provided for a number of insulating compounds characterized by null propagation wavevectors.
Two geometrically frustrated pyrochlore stannates, undergoing long range magnetic order below 1K, were investigated at very low temperature. Anomalies in the behaviour of hyperfine quantities are found, by 155Gd Mossbauer spectroscopy in Gd2Sn2O7 and by low temperature specific heat measurements in Tb2Sn2O7. They are interpreted in terms of fluctuations of the correlated Gd or Tb spins, using a model two-level system (the nuclear spins) submitted to a randomly fluctuating (hyperfine) field.
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