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Register a new userAntiferromagnetic correlations in strongly valence fluctuating CeIrSn
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CeIrSn with a quasikagome Ce lattice in the hexagonal basal plane is a strongly valence fluctuating compound, as we confirm by hard x-ray photoelectron spectroscopy and inelastic neutron scattering, with a high Kondo temperature of $T_{mathrm{K}}sim 480$,K. We report a negative in-plane thermal expansion $alpha/T$ below 2,K, which passes through a broad minimum near 0.75,K. Volume and $a$-axis magnetostriction for $B parallel a$ are markedly negative at low fields and change sign before a sharp metamagnetic anomaly at 6,T. These behaviors are unexpected for Ce-based intermediate valence systems, which should feature positive expansivity. Rather they point towards antiferromagnetic correlations at very low temperatures. This is supported by muon spin relaxation measurements down to 0.1,K, which provide microscopic evidence for a broad distribution of internal magnetic fields. Comparison with isostructural CeRhSn suggests that these antiferromagnetic correlations emerging at $Tll T_{mathrm{K}}$ result from geometrical frustration.
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A central issue in material science is to obtain understanding of the electronic correlations that control complex materials. Such electronic correlations frequently arise due to the competition of localized and itinerant electronic degrees of freedom. While the respective limits of well-localized or entirely itinerant ground states are well-understood, the intermediate regime that controls the functional properties of complex materials continues to challenge theoretical understanding. We have used neutron spectroscopy to investigate plutonium, which is a prototypical material at the brink between bonding and non-bonding configurations. Our study reveals that the ground state of plutonium is governed by valence fluctuations, that is, a quantum-mechanical superposition of localized and itinerant electronic configurations as recently predicted by dynamical mean field theory. Our results not only resolve the long-standing controversy between experiment and theory on plutoniums magnetism, but also suggest an improved understanding of the effects of such electronic dichotomy in complex materials.
We have investigated the optical conductivity of the prominent valence fluctuating compounds EuIr2Si2 and EuNi2P2 in the infrared energy range to get new insights into the electronic properties of valence fluctuating systems. For both compounds we observe upon cooling the formation of a renormalized Drude response, a partial suppression of the optical conductivity below 100 meV and the appearance of a mid-infrared peak at 0.15 eV for EuIr2Si2 and at 0.13 eV for EuNi2P2. Most remarkably, our results show a strong similarity with the optical spectra reported for many Ce- or Yb-based heavy fermion metals and intermediate valence systems, although the phase diagrams and the temperature dependence of the valence differ strongly between Eu- and Ce-/Yb-systems. This suggests that the hybridization between 4f- and conduction electrons, which is responsible for the properties of Ce- and Yb-systems, plays an important role in valence fluctuating Eu-systems.
$alpha$-YbAlB$_4$ is the locally isostructural polymorph of $beta$-YbAlB$_4$, the first example of an Yb-based heavy fermion superconductor which exhibits pronounced non-Fermi-liquid behavior above $T_{rm c}$. Interestingly, both $alpha$-YbAlB$_4$ and $beta$-YbAlB$_4$ have strongly intermediate valence. Our single crystal study of the specific heat, magnetization and resistivity has confirmed the Fermi liquid ground state of $alpha$-YbAlB$_4$ ~in contrast with the quantum criticality observed in $beta$-YbAlB$_4$. Both systems exhibit Kondo lattice behavior with the characteristic temperature scale $T^* sim$ 8 K in addition to a valence fluctuation scale $sim 200$ K. Below $T^*$, $alpha$-YbAlB$_4$ a heavy Fermi liquid state with an electronic specific heat coefficient $gammasim$ 130 mJ/mol K$^2$ and a large Wilson ratio more than 7, which indicates ferromagnetic correlation between Yb moments. A large anisotropy in the resistivity suggests that the hybridization between 4$f$ and conduction electrons is much stronger in the $ab$-plane than along the c-axis. The strongly anisotropic hybridization as well as the large Wilson ratio is the key to understand the unusual Kondo lattice behavior and heavy fermion formation in mixed valent compounds.
X-ray magnetic circular dichroism (XMCD) at the Eu L-edge (2p->5d) in two compounds exhibiting valence fluctuation, namely EuNi2(Si0.18Ge0.82)2 and EuNi2P2, has been investigated at pulsed high magnetic fields of up to 40 T. A distinct XMCD peak corresponding to the trivalent state (Eu3+; f6), whose ground state is nonmagnetic (J=0), was observed in addition to the main XMCD peak corresponding to the magnetic (J=7/2) divalent state (Eu2+; f7). This result indicates that the 5d electrons belonging to both valence states are magnetically polarized. It was also found that the ratio P5d(3+)/P5d(2+) between the polarization of 5d electrons (P5d) in the Eu3+ state and that of Eu2+ is ~ 0.1 in EuNi2(Si0.18Ge0.82)2 and ~ 0.3 in EuNi2P2 at magnetic fields where their macroscopic magnetization values are the same. The possible origin of the XMCD of the Eu3+ state and an explanation of the dependence of P5d(3+)/P5d(2+) on the material are discussed in terms of hybridization between the conduction electrons and the f electrons.
Sb-NMR/NQR study has revealed a formation of a pseudogap at the Fermi level in the density of states in a valence fluctuating compound CeIrSb. The nuclear spin-lattice relaxation rate divided by temperature, 1/T_1T has a maximum around 300 K and decreases significantly as 1/T_1T ~ T^2, followed by a 1/T_1T = const. relation at low temperature. This temperature dependence of 1/T_1T is well reproduced by assuming a V-shaped energy gap with a residual density of states at the Fermi level. The size of energy gap for CeIrSb is estimated to be about 350 K, which is by one order of magnitude larger than those for the isostructural Kondo semiconductors CeRhSb and CeNiSn. Despite the large difference in the size of energy gap, CeIrSb, CeRhSb and CeNiSn are indicated to be classified into the same group revealing a V-shaped gap due to c-f hybridization. The temperature dependence of the Knight shift measured in a high magnetic field agrees with the formation of this pseudogap.
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