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Register a new userCharge, lattice and magnetism across the valence crossover in EuIr$_2$Si$_2$ single crystals
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We present a detailed study of the temperature evolution of the crystal structure, specific heat, magnetic susceptibility and resistivity of single crystals of the paradigmatic valence-fluctuating compound EuIr$_2$Si$_2$. A comparison to stable-valent isostructural compounds EuCo$_2$Si$_2$ (with Eu$^{3+}$), and EuRh$_2$Si$_2$, (with Eu$^{2+}$) reveals an anomalously large thermal expansion indicative of the lattice softening associated to valence fluctuations. A marked broad peak at temperatures around 65-75 K is observed in specific heat, susceptibility and the derivative of resistivity, as thermal energy becomes large enough to excite Eu into a divalent state, which localizes one f electron and increases scattering of conduction electrons. In addition, the intermediate valence at low temperatures manifests in a moderately renormalized electron mass, with enhanced values of the Sommerfeld coefficient in the specific heat and a Fermi-liquid-like dependence of resistivity at low temperatures. The high residual magnetic susceptibility is mainly ascribed to a Van Vleck contribution. Although the intermediate/fluctuating valence duality is to some extent represented in the interconfiguration fluctuation model commonly used to analyze data on valence-fluctuating systems, we show that this model cannot describe the different physical properties of EuIr$_2$Si$_2$ with a single set of parameters.
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We present the crystal growth as well as the structural, chemical and physical chracterization of SmRh$_2$Si$_2$ single crystals. Their ground state is antiferromagnetic, as indicated by the behaviour of the magnetic susceptibility and the specific heat at the second order phase transition observed at T$_{rm N}$ = 64 K. The Sommerfeld coefficient is small and similar to that of LuRh$_2$Si$_2$ with $gamma_0approx$ J/(molK$^2$). Susceptibility measurements show no Curie-Weiss behaviour at high temperatures which is a consequence of the large Van-Vleck contribution of the excited multiplets of Sm$^{3+}$. Previous angle-resolved photoemission studies showed that at 10 K, the valence of the Sm ions is smaller than three at the surface as well as in the bulk, suggesting a possible Kondo screening of the Sm$^{3+}$ ions. This could not be observed in our thermodynamic and transport measurements.
Yb$_2$Si$_2$Al may be a prototype for exploring different aspects of the Shastry-Sutherland lattice, formed by planes of orthogonally coupled Yb ions. Measurements of the magnetic susceptibility find incoherently fluctuating Yb$^{3+}$ moments coexisting with a weakly correlated metallic state that is confirmed by measurements of the electrical resistivity. Increasing signs of Kondo coherence are found with decreasing temperature, including an enhanced Sommerfeld coefficient and Kadowaki-Woods ratio that signal that the metallic state found at the lowest temperatures is a Fermi liquid where correlations have become significantly stronger. A pronounced peak in the electronic and magnetic specific heat indicates that the coupling of the Yb moments to the conduction electrons leads to an effective Kondo temperature that is approximately 30 K. The valence of Yb$_2$Si$_2$Al has been investigated with electron spectroscopy methods. Yb$_2$Si$_2$Al is found to be strongly intermediate valent ($v_F=2.68(2)$ at 80 K). Taken together, these experimental data are consistent with a scenario where a coherent Kondo lattice forms in Yb$_2$Si$_2$Al from an incoherently fluctuating ensemble of Yb moments with incomplete Kondo compensation, and strong intermediate valence character.
Using a combination of Density Functional Theory, mean-field analysis and exact diagonalization calculations we reveal the emergence of a dimerized charge ordered state in TMTTF$_2$-PF$_6$ organic crystal. The interplay between charge and spin order leads to a rich phase diagram. Coexistence of charge ordering with a structural dimerization results in a ferroelectric phase, which has been observed experimentally. The tendency to the dimerization is magnetically driven revealing TMTTF$_2$-PF$_6$ as a multiferroic material.
We report the synthesis and the magnetic properties of single crystalline CeRhAl$_4$Si$_2$ and CeIrAl$_4$Si$_2$ and their non magnetic La-analogs. The single crystals of these quaternary compounds were grown using Al-Si binary eutectic as flux. The anisotropic magnetic properties of the cerium compounds were explored in detail by means of magnetic susceptibility, isothermal magnetization, electrical resistivity, magnetoresistivity and heat capacity measurements. Both CeRhAl$_4$Si$_2$ and CeIrAl$_4$Si$_2$ undergo two antiferromagnetic transitions, first from the paramagnetic to an antiferromagnetic state at $T_{rm N1}$~=~12.6~K and 15.5~K, followed by a second transition at lower temperatures $T_{rm N2}$~=~9.4~K and 13.8~K, respectively. The paramagnetic susceptibility is highly anisotropic and its temperature dependence in the magnetically ordered state suggests the $c$-axis to be the relatively easy axis of magnetization. Concomitantly, isothermal magnetization at 2~K along the $c$-axis shows a sharp spin-flop transition accompanied by a sizeable hysteresis, while it varies nearly linearly with field along the [100] direction up to the highest field 14~T, of our measurement. The electrical resistivity provides evidence of the Kondo interaction in both compounds, inferred from its $-lnT$ behavior in the paramagnetic region. The heat capacity data confirm the bulk nature of the two magnetic transitions in each compound, and further confirm the presence of Kondo interaction by a reduced value of the entropy associated with the magnetic ordering. From the heat capacity data below 1~K, the coefficient of the linear term in the electronic heat capacity, $gamma$, is inferred to be 195.6 and 49.4~mJ/mol K$^2$ in CeRhAl$_4$Si$_2$ and CeIrAl$_4$Si$_2$, respectively classifying these materials as moderate heavy fermion compounds.
We have performed pressure dependent X-ray diffraction and resonant X-ray emission spectroscopy experiments on USb$_2$ to further characterize the AFM-FM transition occurring near 8 GPa. We have found the magnetic transition coincides with a tetragonal to orthorhombic transition resulting in a 17% volume collapse as well as a transient $textit{f}$-occupation enhancement. Compared to UAs$_2$ and UAsS, USb$_2$ shows a reduced bulk modulus and transition pressure and an increased volume collapse at the structural transition. Except for an enhancement across the transition region, the $textit{f}$-occupancy decreases steadily from 1.96 to 1.75.
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