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Evolution of single-ion crystal field and Kondo features in Ce$_{0.5}$La$_{0.5}$Ni$_{9-x}$Cu$_x$Ge$_4$

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 Publication date 2009
  fields Physics
and research's language is English




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Starting with the heavy fermion compound CeNi$_9$Ge$_4$, the substitution of nickel by copper leads to a dominance of the RKKY interaction in competition with the Kondo and crystal field interaction. Consequently, this results in an antiferromagnetic phase transition in CeNi$_{9-x}$Cu$_x$Ge$_4$ for $x>0.4$, which is, however, not fully completed up to a Cu-concentration of $x=1$. To study the influence of single-ion effects on the AFM ordering by shielding the $4f$-moments, we analyzed the spin diluted substitution series La$_{0.5}$Ce$_{0.5}$Ni$_{9-x}$Cu$_x$Ge$_4$ by magnetic susceptibility $chi$ and specific heat $C$ measurements. For small Cu-amounts $xleq 0.4$ the data reveal single-ion scaling with regard to the Ce-concentration, while for larger Cu-concentrations the AFM transition (encountered in the CeNi$_{9-x}$Cu$_x$Ge$_4$ series) is found to be completely depressed. Calculation of the entropy reveal that the Kondo-effect still shields the 4$f$-moments of the Ce$^{3+}$-ions in CeNi$_8$CuGe$_4$.



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CeNi$_{9}$Ge$_4$ exhibits unusual non-Fermi liquid behavior with the largest ever recorded value of the electronic specific heat $Delta C/T cong 5.5$ JK$^{-2}$mol$^{-1}$ without showing any evidence of magnetic order. Specific heat measurements show that the logarithmic increase of the Sommerfeld coefficient flattens off below 200 mK. In marked contrast, the local susceptibility $Deltachi$ levels off well above 200 mK and already becomes constant below 1 K. Furthermore, the entropy reaches 2$R$ln2 below 20 K corresponding to a four level system. An analysis of $C$ and $chi$ was performed in terms of an $SU(N=4)$ single impurity Anderson model with additional crystal electric field (CEF) splitting. Numerical renormalization group calculations point to a possible consistent description of the different low temperature scales in $Delta c$ and $Delta chi$ stemming from the interplay of Kondo effect and crystal field splitting.
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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We demonstrate that the cluster-glass state emerges as ferromagnetic quantum criticality is avoided in itinerant ferromagnet Sr1-x(La0.5K0.5)xRuO3. In this compound, the ferromagnetic order is suppressed by increasing x, and then disappears at the critical concentration: x=0.5. In this x range, the present study reveals that no prominent feature is ascribed to the quantum critical fluctuations in specific heat. Instead, ac magnetic susceptibility exhibits a broad peak due to spontaneous spin freezing, and the peak temperature depends significantly on the frequency of the applied ac magnetic field. Furthermore, specific heat is enhanced within a wide temperature range, whereas specific heat shows no salient anomaly associated with spin freezing. These features are characteristics of the formation of cluster-glass; in particular, the observed frequency variations in ac magnetic susceptibility are well described by the Vogel-Fulcher law. We compare the features concerning the suppression of the ferromagnetic order in this doped compound with those in isostructural Ca- and La-doped SrRuO3, and suggest that a local correlated disorder effect and the very small coherence of itinerant Ru 4d electrons are responsible for the cluster-glass formation instead of the quantum phase transition in Sr1-x(La0.5K0.5)xRuO3.
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