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Register a new userDoping-induced redistribution of magnetic spectral weight in substituted hexaborides Ce$_{1-x}$La$_x$B$_6$ and Ce$_{1-x}$Nd$_x$B$_6$
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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.
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Using Fourier-transform infrared spectroscopy and optical ellipsometry, room temperature spectra of complex conductivity of single crystals of hexaborides Gd$_x$La$_{1-x}$B$_6$, $x$(Gd)$=0$, 0.01, 0.1, 0.78, 1 are determined in the frequency range 30$-$35000$~cm^{-1}$. In all compounds, in addition to the Drude free-carrier spectral component, a broad excitation is discovered with the unusually large dielectric contribution $Delta$$varepsilon$=5000 -- 15000 and non-Lorentzian lineshape. It is suggested that the origin of the excitation is connected with the dynamic cooperative Jahn-Teller effect of B$_6$ clusters. Analysis of the spectra together with the results of DC and Hall resistivity measurements shows that only 30$-$50$%$ of the conduction band electrons are contributing to the free carrier conductivity with the rest being involved in the formation of an overdamped excitation, thus providing possible explanation of remarkably low work function of thermoemission of Gd$_x$La$_{1-x}$B$_6$ and non-Fermi-liquid behavior in GdB$_6$ crystals.
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.
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.
Motivated by the possibility of observing the co-existence between magnetism and unconventional superconductivity in heavy-fermion Ce$_{1-x}$Sm$_x$CoIn$_5$ alloys, we studied how the samarium substitution on the cerium site affects the magnetic field-tuned-quantum criticality of stoicheometric CeCoIn$_5$ by performing specific heat and resistivity measurements. By applying an external magnetic field, we have observed Fermi-liquid to non-Fermi-liquid crossovers in the temperature dependence of the electronic specific heat normalized by temperature and of the resistivity. We obtained the magnetic-field-induced quantum critical point (QCP) by extrapolating to zero temperature the temperature - magnetic field dependence at which the crossovers take place. Furthermore, a scaling analysis of the electronic specific heat is used to confirm the existence of the QCP. We have found that the magnitude of the magnetic-field-induced QCP decreases with increasing samarium concentration. Our analysis of heat capacity and resistivity data reveals a zero-field QCP for $x_textrm{cr} approx 0.15$, which falls inside the region where Sm ions antiferromagnetism and superconductivity co-exist.
We present magnetic susceptibility, resistivity, specific heat, and thermoelectric power measurements on (Ce$_{1-x}$La$_x$)Cu$_2$Ge$_2$ single crystals (0 $leq xleq$ 1). With La substitution, the antiferromagnetic temperature $T_N$ is suppressed in an almost linear fashion and moves below 0.36 K, the base temperature of our measurements for $x>$ 0.8. Surprisingly, in addition to robust antiferromagnetism, the system also shows low temperature coherent scattering below $T_{coh}$ up to $sim$ 0.9 of La, indicating a small percolation limit $sim$ 9$%$ of Ce that separates a coherent regime from a single-ion Kondo impurity regime. $T_{coh}$ as a function of magnetic field was found to have different behavior for $x$< 0.9 and $x$> 0.9. Remarkably, $(T_{coh})^2$ at $H$ = 0 was found to be linearly proportional to $T_N$. The jump in the magnetic specific heat $delta C_{m}$ at $T_N$ as a function of $T_K/T_N$ for (Ce$_{1-x}$La$_x$)Cu$_2$Ge$_2$ follows the theoretical prediction based on the molecular field calculation for the $S$ = 1/2 resonant level model.
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