Subscribe to the gold package and get unlimited access to Shamra Academy
Register a new userUnstable Spin-Ice Order in the Stuffed Metallic Pyrochlore Pr$_{2+x}$Ir$_{2-x}$O$_{7-delta}$
110
0
0.0
(
0
)
Added by
Douglas E. MacLaughlin
Publication date
2015
fields
Physics
and research's language is
English
Ask ChatGPT about the research
No Arabic abstract
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.
rate research
Read More
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.
Magnetic fluctuations induced by geometric frustration of local Ir-spins disturb the formation of long range magnetic order in the family of pyrochlore iridates, R$_{2}$Ir$_{2}$O$_{7}$ (R = lanthanide)$^{1}$. As a consequence, Pr$_{2}$Ir$_{2}$O$_{7}$ lies at a tuning-free antiferromagnetic-to-paramagnetic quantum critical point and exhibits a diverse array of complex phenomena including Kondo effect, biquadratic band structure, metallic spin-liquid (MSL), and anomalous Hall effect$^{2-5}$. Using spectroscopic imaging with the scanning tunneling microscope, complemented with machine learning K-means clustering analysis, density functional theory, and theoretical modeling, we probe the local electronic states in single crystal of Pr$_{2}$Ir$_{2}$O$_{7}$ and discover an electronic phase separation. Nanoscale regions with a well-defined Kondo resonance are interweaved with a non-magnetic metallic phase with Kondo-destruction. Remarkably, the spatial nanoscale patterns display a correlation-driven fractal geometry with power-law behavior extended over two and a half decades, consistent with being in proximity to a critical point. Our discovery reveals a new nanoscale tuning route, viz. using a spatial variation of the electronic potential as a means of adjusting the balance between Kondo entanglement and geometric frustration.
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.
The pyrochlore oxides Dy$_{2}$Ti$_{2}$O$_{7}$ and Ho$_{2}$Ti$_{2}$O$_{7}$ are well studied spin ice systems and have shown the evidences of magnetic monopole excitations. Unlike these, Dy$_{2}$Zr$_{2}$O$_{7}$ is reported to crystallize in a distorted fluorite structure. We present here the magnetic and heat capacity studies of La substituted Dy$_{2}$Zr$_{2}$O$_{7}$. Our findings suggest the absence of spin ice state in Dy$_{2}$Zr$_{2}$O$_{7}$ but the emergence of the magnetic field induced spin freezing near T $approx$ 10 K in ac susceptibility measurements which is similar to Dy$_{2}$Ti$_{2}$O$_{7}$. The magnetic heat capacity of Dy$_{2}$Zr$_{2}$O$_{7}$ shows a shift in the peak position from 1.2 K in zero field to higher temperatures in the magnetic field, with the corresponding decrease in the magnetic entropy. The low temperature magnetic entropy at 5 kOe field is Rln2 - (1/2)Rln(3/2) which is same as for the spin ice state. Substitution of non-magnetic, isovalent La$^{3+}$ for Dy$^{3+}$ gradually induces the structural change from highly disordered fluorite to weakly ordered pyrochlore phase. The La$^{3+}$ substituted compounds with less distorted pyrochlore phase show the spin freezing at lower field which strengthens further on the application of magnetic field. Our results suggest that the spin ice state can be stabilized in Dy$_{2}$Zr$_{2}$O$_{7}$ either by slowing down of the spin dynamics or by strengthening the pyrochlore phase by suitable substitution in the system.
Recent low temperature heat capacity (C$_P$) measurements on polycrystalline samples of the pyrochlore antiferromagnet Tb$_{2+x}$Ti$_{2-x}$O$_{7+delta}$ have shown a strong sensitivity to the precise Tb concentration $x$, with a large anomaly exhibited for $x sim 0.005$ at $T_C sim 0.5$ K and no such anomaly and corresponding phase transition for $x le 0$. We have grown single crystal samples of Tb$_{2+x}$Ti$_{2-x}$O$_{7+delta}$, with approximate composition $x=-0.001, +0.0042$, and $+0.0147$, where the $x=0.0042$ single crystal exhibits a large C$_P$ anomaly at $T_C$=0.45 K, but neither the $x=-0.001$ nor the $x=+0.0147$ single crystals display any such anomaly. We present new time-of-flight neutron scattering measurements on the $x=-0.001$ and the $x=+0.0147$ samples which show strong $left(frac{1}{2},frac{1}{2},frac{1}{2}right)$ quasi-Bragg peaks at low temperatures characteristic of short range antiferromagnetic spin ice (AFSI) order at zero magnetic field but only under field-cooled conditions, as was previously observed in our $x = 0.0042$ single crystal. These results show that the strong $left(frac{1}{2},frac{1}{2},frac{1}{2}right)$ quasi-Bragg peaks and gapped AFSI state at low temperatures under field cooled conditions are robust features of Tb$_2$Ti$_2$O$_7$, and are not correlated with the presence or absence of the C$_P$ anomaly and phase transition at low temperatures. Further, these results show that the ordered state giving rise to the C$_P$ anomaly is confined to $0 leq x leq 0.01$ for Tb$_{2+x}$Ti$_{2-x}$O$_{7+delta}$, and is not obviously connected with conventional order of magnetic dipole degrees of freedom.
Log in to be able to interact and post comments
comments
Fetching comments
Sign in to be able to follow your search criteria
