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Nd2Sn2O7: an all-in-all-out pyrochlore magnet with no divergence-free field and anomalously slow paramagnetic spin dynamics

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




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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. The 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.



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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.
We report the low temperature magnetic properties of Nd$^{3+}$ pyrochlore $rm Nd_2ScNbO_7$. Susceptibility and magnetization show an easy-axis moment, and heat capacity reveals a phase transition to long range order at $T_N=371(2)$ mK with a fully recovered $Delta S = R ln(2)$, 53% of it recovered for $T>T_N$. Elastic neutron scattering shows a long-range all-in-all-out magnetic order with low-$Q$ diffuse elastic scattering. Inelastic neutron scattering shows a low-energy flat-band, indicating a magnetic Hamiltonian similar to $rm Nd_2Zr_2O_7$. Nuclear hyperfine excitations measured by ultra-high-resolution neutron backscattering indicates a distribution of static electronic moments below $T_N$, which may be due to B-site disorder influencing Nd crystal electric fields. Analysis of heat capacity data shows an unexpected $T$-linear or $T^{3/2}$ term which is inconsistent with conventional magnon quasiparticles, but is consistent with fractionalized spinons or gapless local spin excitations. We use legacy data to show similar behavior in $rm Nd_2Zr_2O_7$. Comparing local static moments also reveals a suppression of the nuclear Schottky anomaly in temperature, evidencing a fraction of Nd sites with nearly zero static moment, consistent with exchange-disorder-induced random singlet formation. Taken together, these measurements suggest an unusual fluctuating magnetic ground state which mimics a spin-liquid -- but may not actually be one.
Dimensionality and symmetry play deterministic roles in the laws of Nature. They are important tools to characterize and understand quantum phase transitions, especially in the limit of strong correlations between spin, orbit, charge, and structural degrees of freedom. Using newly-developed, high-pressure resonant x-ray magnetic and charge diffraction techniques, we have discovered a quantum critical point in Cd2Os2O7 as the all-in-all-out (AIAO) antiferromagnetic order is continuously suppressed to zero temperature and, concomitantly, the cubic lattice structure continuously changes from space group Fd-3m to F-43m. Surrounded by three phases of different time reversal and spatial inversion symmetries, the quantum critical region anchors two phase lines of opposite curvature, with striking departures from a mean-field form at high pressure. As spin fluctuations, lattice breathing modes, and quasiparticle excitations interact in the quantum critical region, we argue that they present the necessary components for strongly-coupled quantum criticality in this three-dimensional compound.
155 - Z. Hiroi , J. Yamaura , T. Hirose 2015
We investigate the metal-insulator transition (MIT) of the osmium pyrochlore oxide Cd2Os2O7 through transport and magnetization measurements. The MIT and a magnetic transition to the all-in/all-out (AIAO) order occur simultaneously at 227 K. We propose a mechanism based on a Lifshitz transition induced by the AIAO magnetic order probably via strong spin-orbit couplings in the specific semimetallic band structure. It is suggested, moreover, that two observed puzzles, a finite conductivity near T = 0 and an emergence of weak ferromagnetic moments, are not bulk properties but originate at magnetic domain walls between two kinds of AIAO domains.
Nd2Hf2O7, belonging to the family of geometrically frustrated cubic rare earth pyrochlore oxides, was recently identified to order antiferromagnetically below T_N = 0.55 K with an all-in/all-out arrangement of Nd3+ moments, however with a much reduced ordered state moment. Herein we investigate the spin dynamics and crystal field states of Nd2Hf2O7 using muon spin relaxation (muSR) and inelastic neutron scattering (INS) measurements. Our muSR study confirms the long range magnetic ordering and shows evidence for coexisting persistent dynamic spin fluctuations deep inside the ordered state down to 42 mK. The INS data show the crytal electric field (CEF) excitations due to the transitions both within the ground state multiplet and to the first excited state multiplet. The INS data are analyzed by a model based on CEF and crystal field states are determined. Strong Ising-type anisotropy is inferred from the ground state wavefunction. The CEF parameters indicate the CEF-split Kramers doublet ground state of Nd3+ to be consistent with the dipolar-octupolar character.
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