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Register a new userMuon spin relaxation and hyperfine-enhanced 141Pr nuclear spin dynamic in Pr(Os,Ru)4Sb12 and (Pr,La)Os4Sb12
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Zero- and longitudinal-field muon spin relaxation (MuSR) experiments have been carried out in the alloy series Pr(Os1-xRux)4Sb12 and Pr1-yLayOs4Sb12 to elucidate the anomalous dynamic muon spin relaxation observed in these materials. The damping rate associated with this relaxation varies with temperature, applied magnetic field, and dopant concentrations x and y in a manner consistent with the ``hyperfine enhancement of 141Pr nuclear spins first discussed by Bleaney in 1973. This mechanism arises from Van Vleck-like admixture of magnetic Pr3+ crystalline-electric-field-split excited states into the nonmagnetic singlet ground state by the nuclear hyperfine coupling, thereby increasing the strengths of spin-spin interactions between 141Pr and muon spins and within the 141Pr spin system. We find qualitative agreement with this scenario, and conclude that electronic spin fluctuations are not directly involved in the dynamic muon spin relaxation.
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Positive-muon ($mu^+$) Knight shifts have been measured in the paramagnetic states of Pr$_{1-x}$Nd$_x$Os$_4$Sb$_{12}$ alloys, where $x =$ 0, 0.25, 0.45, 0.50, 0.55, 0.75, and 1.00. In Pr-substituted NdOs$_4$Sb$_{12}$ ($x le$ 0.75), but not in NdOs$_4$Sb$_{12}$, Clogston-Jaccarino plots of $mu^+$ Knight shift~$K$ versus magnetic susceptibility~$chi$ exhibit an anomalous saturation of $K(chi)$ at $sim-$0.5% for large susceptibilities (low temperatures), indicating a reduction of the coupling strength between $mu^+$ spins and $4f$ paramagnetism for temperatures $lesssim$ 15~K. We speculate that itinerant Pr$^{3+}$ quadrupolar excitations, invoked to mediate the superconducting Cooper-pair interaction, might modify the $mu^+$-$4f$ ion indirect spin-spin interaction.
Muon spin rotation and relaxation ($mu$SR) experiments have been carried out to characterize magnetic and superconducting ground states in the Pr$_{1-x}$Nd$_x$Os$_4$Sb$_{12}$ alloy series. In the ferromagnetic end compound NdOs$_4$Sb$_{12}$ the spontaneous local field at positive-muon ($mu^+$) sites below the ordering temperature $T_C$ is greater than expected from dipolar coupling to ferromagnetically aligned Nd$^{3+}$ moments, indicating an additional indirect RKKY-like transferred hyperfine mechanism. For 0.45 $le x le$ 0.75, $mu^+$ spin relaxation rates in zero and weak longitudinal applied fields indicate that static fields at $mu^+$ sites below $T_C$ are reduced and strongly disordered. We argue this is unlikely to be due to reduction of Nd$^{3+}$ moments, and speculate that the Nd$^{3+}$-$mu^+$ interaction is suppressed and disordered by Pr doping. In an $x$ = 0.25 sample, which is superconducting below $T_c$ = 1.3 K, there is no sign of spin freezing (static Nd$^{3+}$ magnetism), ordered or disordered, down to 25 mK. Dynamic $mu^+$ spin relaxation is strong, indicating significant Nd-moment fluctuations. The $mu^+$ diamagnetic frequency shift and spin relaxation in the superconducting vortex-lattice phase decrease slowly below $T_c$, suggesting pair breaking and/or possible modification of Fermi-liquid renormalization by Nd spin fluctuations. For 0.25 $le x le$ 0.75, the $mu$SR data provide evidence against phase separation; superconductivity and Nd$^{3+}$ magnetism coexist on the atomic scale.
Zero-field muon spin relaxation experiments have been carried out in the Pr(Os_{1-x}Ru_x)_4Sb_12 and Pr_{1-y}La_yOs_4Sb_12 alloy systems to investigate broken time-reversal symmetry (TRS) in the superconducting state, signaled by the onset of a spontaneous static local magnetic field B_s. In both alloy series B_s initially decreases linearly with solute concentration. Ru doping is considerably more efficient than La doping, with a ~50% faster initial decrease. The data suggest that broken TRS is suppressed for Ru concentration x >~ 0.6, but persists for essentially all La concentrations. Our data support a crystal-field excitonic Cooper pairing mechanism for TRS-breaking superconductivity.
The Pr-rich end of the alloy series Pr$_{1-x}$Nd$_x$Os$_4$Sb$_{12}$ has been studied using muon spin rotation and relaxation. The end compound PrOs$_4$Sb$_{12}$ is an unconventional heavy-fermion superconductor, which exhibits a spontaneous magnetic field in the superconducting phase associated with broken time-reversal symmetry. No spontaneous field is observed in the Nd-doped alloys for x $>$ 0.05. The superfluid density is insensitive to Nd concentration, and no Nd$^{3+}$ static magnetism is found down to the lowest temperatures of measurement. Together with the slow suppression of the superconducting transition temperature with Nd doping, these results suggest anomalously weak coupling between Nd spins and conduction-band states.
The nature of multipolar order and hyperfine-enhanced (HE) $^{141}$Pr nuclear spin dynamics in PrV$_2$Al$_{20}$ was investigated using the muon spin relaxation technique. No explicit sign of time-reversal symmetry breaking was found below the multipolar order temperature $T_Qsim 0.6$ K in a zero applied field as anticipated on the basis of the antiferroquadrupolar (AFQ) order picture proposed by Sakai and Nakatsuji [J. Phys. Soc. Jpn. 80, 063701 (2011)]. Further evidence of the nonmagnetic ground state was obtained from the observation of HE $^{141}$Pr nuclear spin fluctuations in the MHz scale. A marked increase in the muon spin-lattice relaxation rate (1/$T_{rm 1,mu}$) was observed below 1 K with decreasing temperature, which was attributed to the perturbation on the HE $^{141}$Pr nuclear spin dynamics associated with the development of AFQ correlations. The longitudinal field dependence of 1/$T_{rm 1,mu}$ revealed that the enhanced $^{141}$Pr nuclear spin accidentally has an effective gyromagnetic ratio close to that of the muon.
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