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Register a new userCoexisting Magnetic Order and Cooperative Paramagnetism in the Stuffed Pyrochlore Tb_{2+x}Ti_{2-2x}Nb_xO_7
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Neutron scattering and magnetization measurements have been performed on the stuffed pyrochlore system Tb2+xTi2-2xNbxO7. We find that despite the introduction of chemical disorder and increasingly antiferromagnetic interactions, a spin glass transition does not occur for T >= 1.5 K and cooperative paramagnetic behavior exists for all x. For x = 1, Tb3NbO7, an antiferromagnetically ordered state coexisting with cooperative paramagnetic behavior is seen without applying any external fields or pressure, a situation advantageous for studying this cooperative behavior.
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Specific heat, elastic neutron scattering, and muon spin rotation ($mu$SR) experiments have been carried out on a well-characterized sample of stuffed (Pr-rich) Pr$_{2+x}$Ir$_{2-x}$O$_{7-delta}$. Elastic neutron scattering shows the onset of long-range spin-ice 2-in/2-out magnetic order at $T_M = 0.93$ K, with an ordered moment of 1.7(1)$mu_mathrm{B}$/Pr ion at low temperatures. Approximate lower bounds on the correlation length and correlation time in the ordered state are 170 AA and 0.7 ns, respectively. $mu$SR experiments yield an upper bound 2.6(7) mT on the local field $B_mathrm{loc}^{4f}$ at the muon site, which is nearly two orders of magnitude smaller than the expected dipolar field for long-range spin-ice ordering of 1.7$mu_B$ moments (120--270 mT, depending on muon site). This shortfall is due in part to splitting of the non-Kramers crystal-field ground-state doublets of near-neighbor Pr$^{3+}$ ions by the $mu^+$-induced lattice distortion. For this to be the only effect, however, $sim$160 Pr moments out to a distance of $sim$14 AA must be suppressed. An alternative scenario, which is consistent with the observed reduced nuclear hyperfine Schottky anomaly in the specific heat, invokes slow correlated Pr-moment fluctuations in the ordered state that average $B_mathrm{loc}^{4f}$ on the $mu$SR time scale (${sim}10^{-7}$ s), but are static on the time scale of the elastic neutron scattering experiments (${sim}10^{-9}$ s). In this picture the dynamic muon relaxation suggests a Pr$^{3+}$ $4f$ correlation time of a few nanoseconds, which should be observable in a neutron spin echo experiment.
The consequences of nonmagnetic-ion dilution for the pyrochlore family Y$_{2}$($M_{1-x}N_{x}$)$_{2}$O$_{7}$ ($M$ = magnetic ion, $N$ = nonmagnetic ion) have been investigated. As a first step, we experimentally examine the magnetic properties of Y$_{2}$CrSbO$_{7}$ ($x$ = 0.5), in which the magnetic sites (Cr$^{3+}$) are percolative. Although the effective Cr-Cr spin exchange is ferromagnetic, as evidenced by a positive Curie-Weiss temperature, $Theta_mathrm{{CW}}$ = 20.1(6) K, our high-resolution neutron powder diffraction measurements detect no sign of magnetic long range order down to 2 K. In order to understand our observations, we performed numerical simulations to study the bond-disorder introduced by the ionic size mismatch between $M$ and $N$. Based on these simulations, bond-disorder ($x_{b}$ $simeq$ 0.23) percolates well ahead of site-disorder ($x_{s}$ $simeq$ 0.61). This model successfully reproduces the critical region (0.2 < $x$ < 0.25) for the Neel to spin glass phase transition in Zn(Cr$_{1-x}$Ga$_{x}$)$_{2}$O$_{4}$, where the Cr/Ga-sublattice forms the same corner-sharing tetrahedral network as the $M/N$-sublattice in Y$_{2}$($M_{1-x}N_{x}$)$_{2}$O$_{7}$, and the rapid drop in magnetically ordered moment in the Neel phase [Lee $et$ $al$, Phys. Rev. B 77, 014405 (2008)]. Our study stresses the nonnegligible role of bond-disorder on magnetic frustration, even in ferromagnets.
We study the magnetic structure of the stuffed (Tb-rich) pyrochlore iridate Tb$_{2+x}$Ir$_{2-x}$O$_{7-y}$, using resonant elastic x-ray scattering (REXS). In order to disentangle contributions from Tb and Ir magnetic sublattices, experiments were performed at the Ir $L_3$ and Tb $M_5$ edges, which provide selective sensitivity to Ir $5d$ and Tb $4f$ magnetic moments, respectively. At the Ir $L_3$ edge, we found the onset of long-range ${bf k}={bf 0}$ magnetic order below $T_{N}^text{Ir}sim$ 71 K, consistent with the expected signal of all-in all-out (AIAO) magnetic order. Using a single-ion model to calculate REXS cross-sections, we estimate an ordered magnetic moment of $mu_{5d}^{text{Ir}} approx 0.34(3),mu_B$ at 5 K. At the Tb $M_5$ edge, long-range ${bf k}={bf 0}$ magnetic order appeared below $sim40$ K, also consistent with an AIAO magnetic structure on the Tb site. Additional insight into the magnetism of the Tb sublattice is gleaned from measurements at the $M_5$ edge in applied magnetic fields up to 6 T, which is found to completely suppress the Tb AIAO magnetic order. In zero applied field, the observed gradual onset of the Tb sublattice magnetisation with temperature suggests that it is induced by the magnetic order on the Ir site. The persistence of AIAO magnetic order, despite the greatly reduced ordering temperature and moment size compared to stoichiometric Tb$_{2}$Ir$_{2}$O$_{7}$, for which $T_{N}^{text{Ir}} =130$ K and $mu_{5d}^{text{Ir}}=0.56,mu_B$, indicates that stuffing could be a viable means of tuning the strength of electronic correlations, thereby potentially offering a new strategy to achieve topologically non-trivial band crossings in pyrochlore iridates.
The nature of the magnetic transition of the half-filled triangular antiferromagnet Ag$_{2}$NiO$_2$ with $T_{rm N}$=56K was studied with positive muon-spin-rotation and relaxation ($mu^+$SR) spectroscopy. Zero field $mu^+$SR measurements indicate the existence of a static internal magnetic field at temperatures below $T_{rm N}$. Two components with slightly different precession frequencies and wide internal-field distributions suggest the formation of an incommensurate antiferromagnetic order below 56 K. This implies that the antifrerromagnetic interaction is predominant in the NiO$_2$ plane in contrast to the case of the related compound NaNiO$_2$. An additional transition was found at $sim$22 K by both $mu^+$SR and susceptibility measurements. It was also clarified that the transition at $sim$260 K observed in the susceptibility of Ag$_{2}$NiO$_{2}$ is induced by a purely structural transition.
We report a magnetic force microscopy study of the magnetic domain evolution in the layered manganite La$_{2-2x}$Sr$_{1+2x}$Mn$_2$O$_7$ (with $x=0.32$). This strongly correlated electron compound is known to exhibit a wide range of magnetic phases, including a recently uncovered biskyrmion phase. We observe a continuous transition from dendritic to stripe-like domains, followed by the formation of magnetic bubbles due to a field- and temperature dependent competition between in-plane and out-of-plane spin alignments. The magnetic bubble phase appears at comparable field- and temperature ranges as the biskyrmion phase, suggesting a close relation between both phases. Based on our real-space images we construct a temperature-field phase diagram for this composition.
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