No Arabic abstract
Cubic f-electron compounds commonly exhibit highly anisotropic magnetic phase diagrams consisting of multiple long-range ordered phases. Field-driven metamagnetic transitions between them may depend not only on the magnitude, but also on the direction of the applied magnetic field. Examples of such behavior are plentiful among rare-earth borides, such as RB$_6$ or RB$_{12}$ ($R$ = rare earth). In this work, for example, we use torque magnetometry to measure anisotropic field-angular phase diagrams of La-doped cerium hexaborides, Ce$_{1-x}$La$_x$B$_6$ ($x$ = 0, 0.18, 0.28, 0.5). One expects that field-directional anisotropy of phase transitions must be impossible to understand without knowing the magnetic structures of the corresponding competing phases and being able to evaluate their precise thermodynamic energy balance. However, this task is usually beyond the reach of available theoretical approaches, because the ordered phases can be noncollinear, possess large magnetic unit cells, involve higher-order multipoles of 4f ions rather than simple dipoles, or just lack sufficient microscopic characterization. Here we demonstrate that the anisotropy under field rotation can be qualitatively understood on a much more basic level of theory, just by considering the crystal-electric-field scheme of a pair of rare-earth ions in the lattice, coupled by a single nearest-neighbor exchange interaction. Transitions between different crystal-field ground states, calculated using this minimal model for the parent compound CeB6, possess field-directional anisotropy that strikingly resembles the experimental phase diagrams. This implies that the anisotropy of phase transitions is of local origin and is easier to describe than the ordered phases themselves.
We investigate the doping-induced changes in the electronic structure of CeB$_6$ on a series of substituted Ce$_{1-x}R_x$B$_6$ samples ($R$ = La, Nd) using diffuse neutron scattering. We observe a redistribution of magnetic spectral weight across the Brillouin zone, which we associate with the changes in the Fermi-surface nesting properties related to the modified charge carrier concentration. In particular, a strong diffuse peak at the corner of the Brillouin zone ($R$ point), which coincides with the propagation vector of the elusive antiferroquadrupolar (AFQ) order in CeB$_6$, is rapidly suppressed by both La and Nd doping, like the AFQ order itself. The corresponding spectral weight is transferred to the $X(00frac{1}{2})$ point, ultimately stabilizing a long-range AFM order at this wave vector at the Nd-rich side of the phase diagram. At an intermediate Nd concentration, a broad diffuse peak with multiple local maxima of intensity is observed around the $X$ point, evidencing itinerant frustration that gives rise to multiple ordered phases for which Ce$_{1-x}$Nd$_x$B$_6$ is known. On the La-rich side of the phase diagram, however, dilution of the magnetic moments prevents the formation of a similar $(00frac{1}{2})$-type order despite the presence of nesting. Our results demonstrate how diffuse neutron scattering can be used to probe the nesting vectors in complex f-electron systems directly, without reference to the single-particle band structure, and emphasize the role of Fermi surface geometry in stabilizing magnetic order in rare-earth hexaborides.
CeB(6) is a model compound exhibiting antiferroquadrupolar (AFQ) order, its magnetic properties being typically interpreted within localized models. More recently, the observation of strong and sharp magnetic exciton modes forming in its antiferromagnetic (AFM) state at both ferromagnetic and AFQ wave vectors suggested a significant contribution of itinerant electrons to the spin dynamics. Here we investigate the evolution of the AFQ excitation upon the application of an external magnetic field and the substitution of Ce with non-magnetic La, both parameters known to suppress the AFM phase. We find that the exciton energy decreases proportionally to T_N upon doping. In field, its intensity is suppressed, while its energy remains constant. Its disappearance above the critical field of the AFM phase is preceded by the formation of two modes, whose energies grow linearly with magnetic field upon entering the AFQ phase. These findings suggest a crossover from itinerant to localized spin dynamics between the two phases, the coupling to heavy-fermion quasiparticles being crucial for a comprehensive description of the magnon spectrum.
Double-perovskite oxides that contain both 3d and 5d transition metal elements have attracted growing interest as they provide a model system to study the interplay of strong electron interaction and large spin-orbit coupling (SOC). Here, we report on experimental and theoretical studies of the magnetic and electronic properties of double-perovskites (La$_{1-x}$Sr$_x$)$_2$CuIrO$_6$ ($x$ = 0.0, 0.1, 0.2, and 0.3). The undoped La$_2$CuIrO$_6$ undergoes a magnetic phase transition from paramagnetism to antiferromagnetism at T$_N$ $sim$ 74 K and exhibits a weak ferromagnetic behavior below $T_C$ $sim$ 52 K. Two-dimensional magnetism that was observed in many other Cu-based double-perovskites is absent in our samples, which may be due to the existence of weak Cu-Ir exchange interaction. First-principle density-functional theory (DFT) calculations show canted antiferromagnetic (AFM) order in both Cu$^{2+}$ and Ir$^{4+}$ sublattices, which gives rise to weak ferromagnetism. Electronic structure calculations suggest that La$_2$CuIrO$_6$ is an SOC-driven Mott insulator with an energy gap of $sim$ 0.3 eV. Sr-doping decreases the magnetic ordering temperatures ($T_N$ and $T_C$) and suppresses the electrical resistivity. The high temperatures resistivity can be fitted using a variable-range-hopping model, consistent with the existence of disorders in these double-pervoskite compounds.
The field-induced transition in one-dimensional S=1 Heisenberg antiferromagnet with single-ion anisotropy in the presence of a transverse magnetic field is obtained on the basis of the Schwinger boson mean-field theory. The behaviors of the specific heat and susceptibility as functions of temperature as well as the applied transverse field are explored, which are found to be different from the results obtained under a longitudinal field. The anomalies of the specific heat at low temperatures, which might be an indicative of a field-induced transition from a Luttinger liquid phase to an ordered phase, are explicitly uncovered under the transverse field. A schematic phase diagram is proposed. The theoretical results are compared with experimental observations.
We report the results of ac and dc magnetization (M) and heat-capacity (C) measurements on the solid solution, Sr$_3$Cu$_{1-x}$Zn$_x$IrO$_6$. While the Zn end member is known to form in a rhombohedral pseudo one-dimensional K$_4$CdCl$_6$ structure with an antiferromagnetic ordering temperature of (T$_N$ =) 19 K, the Cu end member has been reported to form in a monoclinically distorted form with a Curie temperature of (T$_C$ =) 19 K. The magnetism of the Zn compound is found to be robust to synthetic conditions and is broadly consistent with the behavior known in the literature. However, we find a lower magnetic ordering temperature (T$_o$) for our Cu compound (~ 13 K), thereby suggesting that T$_o$ is sensitive to synthetic conditions. The Cu sample appears to be in a spin-glass-like state at low temperatures, judged by a frequency dependence of ac magnetic susceptibility and a broadening of the C anomaly at the onset of magnetic ordering, in sharp contrast to earlier proposals. Small applications of magnetic field, however, drive this system to ferromagnetism as inferred from the M data. Small substitutions for Cu/Zn (x = 0.75 or 0.25) significantly depress magnetic ordering; in other words, T$_o$ varies non-monotonically with x (T$_o$ ~ 6, 3 and 4 K for x = 0.25, 0.5, and 0.67 respectively). The plot of inverse susceptibility versus temperature is non-linear in the paramagnetic state as if correlations within (or among) the magnetic chains continuously vary with temperature. The results establish