No Arabic abstract
The magnetoresistance (MR) $Delta rho/rho$ of cage-glass compound Ho$_x$Lu$_{1-x}$B$_{12}$ with various concentration of magnetic holmium ions ($x$$leq$0.5) has been studied in detail concurrently with magnetization M(T) and Hall effect investigations on high quality single crystals at temperatures 1.9-120 K and in magnetic field up to 80 kOe. The undertaken analysis of $Deltarho/rho$ allows us to conclude that the large negative magnetoresistance (nMR) observed in vicinity of Neel temperature is caused by scattering of charge carriers on magnetic clusters of Ho$^{3+}$ ions, and that these nanosize regions with AF exchange inside may be considered as short range order AF domains. It was shown that the Yosida relation $-Delta rho/rho$$sim$$M^2$ provides an adequate description of the nMR effect for the case of Langevin type behavior of magnetization. Moreover, a reduction of Ho-ion effective magnetic moments in the range 3-9$mu_B$ was found to develop both with temperature lowering and under the increase of holmium content. A phenomenological description of the large positive quadratic contribution $Delta rho/rho$$sim$$mu_D^2 H^2$ which dominates in Ho$_x$Lu$_{1-x}$B$_{12}$ in the intermediate temperature range 20-120 K allows to estimate the drift mobility exponential changes $mu_D$$sim$$T^{-a}$ with $a$=1.3-1.6 depending on Ho concentration. An even more comprehensive behavior of magnetoresistance has been found in the AF state of Ho$_x$Lu$_{1-x}$B$_{12}$ where an additional linear positive component was observed and attributed to charge carriers scattering on the spin density wave (SDW). High precision measurements of $Deltarho/rho=f(H,T)$ have allowed us also to reconstruct the magnetic H-T phase diagram of Ho$_{0.5}$Lu$_{0.5}$B$_{12}$ and to resolve its magnetic structure as a superposition of 4f (based on localized moments) and 5d (based on SDW) components.
Based on low temperature resistivity, heat capacity and magnetization investigations we show that the unusually strong suppression of superconductivity in Lu$_x$Zr$_{1-x}$B$_{12}$ BSC-type superconductors in the range $x$$<$0.08 is caused by the emergence of static spin polarization in the vicinity of non-magnetic lutetium impurities. The analysis of received results points to a formation of static magnetic moments with $mu_{eff}$$approx$$3mu_B$ per Lu-ion. The size of these spin polarized nanodomains was estimated to be about 5 ${AA}$.
We have investigated the electronic structure of Na$_x$Ca$_{1-x}$Cr$_2$O$_4$ using x-ray absorption spectroscopy together with Anderson impurity model calculations with full multiplets. We show Na$_x$Ca$_{1-x}$Cr$_2$O$_4$ taking a novel mixed-valence electronic state in which the positive charge-transfer (CT) and the negative self-doped states coexist. While CaCr$_2$O$_4$ (one end member) exhibits a typical CT nature with strong covalent character, Na substitution causes a self-doped state with an oxygen hole. In NaCr$_2$O$_4$ (the other end member), positive CT and negative self-doped states coexist with equal weight. This unusual electronic state is in sharp contrast to the conventional mixed-valence description, in which the ground state can be described by the mixture of Cr$^{3+}$ ($3d^3$) and Cr$^{4+}$ ($3d^2$).
We have determined the superconducting and magnetic properties of four samples of Lu$_x$Zr$_{1-x}$B$_{12}$ ($x=0.04$, $0.07$, $0.17$, and $0.8$) using muon spin rotation ($mu$SR) and magnetometry measurements. We observed a strong magnetic signal in both the $mu$SR and magnetometry data in one sample ($x=0.07$), likely caused by the formation of static moments of size $approx 1,mu_{rm B}$ due to a clustering effect of the Lu$^{3+}$ ions. In all other samples, we find only a small magnetic signal in the $mu$SR data thought to originate from boron nuclei in the B$_{12}$ cages. The superconductivity is found to evolve with $x$, with a decrease in $x$ resulting in an increase in critical temperature and a decrease of the penetration depth. Most remarkably, we find the formation of nodes in the superconducting gap for $x leq 0.17$, providing a new example of an $s$-to-$d$-wave crossover in a superconductor.
Lutetium dodecaboride LuB12 is a simple weak-coupling BCS superconductor with critical temperature Tc = 0.42 K, whilst ZrB12 is a strong-coupling BCS superconductor with the highest critical temperature Tc = 6.0 K among this group of materials. In case of lutetium substitution by zirconium ions in LuB12 the crossover from weak- to strong-coupling superconductor can be studied. We have investigated the evolution of critical temperature Tc and critical field Hc in high-quality single crystalline superconducting samples of Lu(1-x)Zr(x)B12 (0 =< x =< 0.45) by measuring magnetic ac susceptibility between 1 K and 50 mK. To obtain this kind of experimental data, a new susceptometer was designed, constructed and tested, which can work in a wide temperature range of 0.05 K - 3 K in 3He-4He dilution refrigerator. The measurements with this new susceptometer revealed how Tc(x) and Hc(x) increases with increasing concentration of zirconium in Lu(1-x)Zr(x)B12 solid solutions as well as how their superconducting phase diagram develops.
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.