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Reduction of the ordered-magnetic moment and its relationship to Kondo coherence in Ce$_{1-x}$La$_{x}$Cu$_{2}$Ge$_{2}$

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 Added by Benjamin Ueland
 Publication date 2017
  fields Physics
and research's language is English




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The microscopic details of the suppression of antiferromagnetic order in the Kondo-lattice series Ce$_{1-x}$La$_{x}$Cu$_{2}$Ge$_{2}$ due to nonmagnetic dilution by La are revealed through neutron diffraction results for $x=0.20$, $0.40$, $0.75$, and $0.85$. Magnetic Bragg peaks are found for $0.20le xle0.75$, and both the N{e}el temperature, $T_{textrm{N}}$, and the ordered magnetic moment per Ce, $mu$, linearly decrease with increasing $x$. The reduction in $mu$ points to strong hybridization of the increasingly diluted Ce $4f$ electrons, and we find a remarkable quadratic dependence of $mu$ on the Kondo-coherence temperature. We discuss our results in terms of local-moment- versus itinerant-type magnetism and mean-field theory, and show that Ce$_{1-x}$La$_{x}$Cu$_{2}$Ge$_{2}$ provides an exceptional opportunity to quantitatively study competing magnetic interactions in a Kondo lattice.

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We report specific heat and neutron scattering experiments performed on the system Ce$_{1-x}$La$_{x}$Ru$_{2}$Si$_{2}$ on the magnetic side of its quantum critical phase diagram. The Kondo temperature does not vanish at the quantum phase transition and elastic scattering indicates a gradual localisation of the magnetism when $x$ increases in the ordered phase.
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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The evolution of the thermopower EuCu{2}(Ge{1-x}Si{x}){2} intermetallics, which is induced by the Si-Ge substitution, is explained by the Kondo scattering of conduction electrons on the Eu ions which fluctuate between the magnetic 2+ and non-magnetic 3+ Hunds rule configurations. The Si-Ge substitution is equivalent to chemical pressure which modifies the coupling and the relative occupation of the {it f} and conduction states.
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In mixed-valence or heavy-fermion systems, the hybridization between local $f$ orbitals and conduction band states can cause the suppression of long-range magnetic order, which competes with strong spin fluctuations. Ce- and Yb-based systems have been found to exhibit fascinating physical properties (heavy-fermion superconductivity, non-Fermi-liquid states, etc.) when tuned to the vicinity of magnetic quantum critical points by use of various external control parameters (temperature, magnetic field, chemical composition). Recently, similar effects (mixed-valence, Kondo fluctuations, heavy Fermi liquid) have been reported to exist in some Eu-based compounds. Unlike Ce (Yb), Eu has a multiple electron (hole) occupancy of its $4f$ shell, and the magnetic Eu$^{2+}$ state ($4f^7$) has no orbital component in the usual $LS$ coupling scheme, which can lead to a quite different and interesting physics. In the EuCu$_{2}$(Si$_{x}$Ge$_{1-x}$)$_{2}$ series, where the valence can be tuned by varying the Si/Ge ratio, it has been reported that a significant valence fluctuation can exist even in the magnetic order regime. This paper presents a detailed study of the latter material using different microscopic probes (XANES, Mossbauer spectroscopy, elastic and inelastic neutron scattering), in which the composition dependence of the magnetic order and dynamics across the series is traced back to the change in the Eu valence state. In particular, the results support the persistence of valence fluctuations into the antiferromagnetic state over a sizable composition range below the critical Si concentration $x_c approx 0.65$. The sequence of magnetic ground states in the series is shown to reflect the evolution of the magnetic spectral response.
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