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Register a new userOptical Evidence of Itinerant-Localized Crossover of $4f$ Electrons in Cerium Compounds
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Cerium (Ce)-based heavy-fermion materials have a characteristic double-peak structure (mid-IR peak) in the optical conductivity [$sigma(omega)$] spectra originating from the strong conduction ($c$)--$f$ electron hybridization. To clarify the behavior of the mid-IR peak at a low $c$-$f$ hybridization strength, we compared the $sigma(omega)$ spectra of the isostructural antiferromagnetic and heavy-fermion Ce compounds with the calculated unoccupied density of states and the spectra obtained from the impurity Anderson model. With decreasing $c$-$f$ hybridization intensity, the mid-IR peak shifts to the low-energy side owing to the renormalization of the unoccupied $4f$ state, but suddenly shifts to the high-energy side owing to the $f$-$f$ on-site Coulomb interaction at a slight localized side from the quantum critical point (QCP). This finding gives us information on the change in the electronic structure across QCP.
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The electronic properties of Cerium (Ce) and ytterbium (Yb) intermetallic compounds may display a more local or more itinerant character depending on the interplay of the exchange interactions among the $4f$ electrons and the Kondo coupling between $4f$ and conduction electrons. For the more itinerant case, the materials form heavy-fermions once the Kondo effect is developed at low temperatures. Hence, a temperature variation occurs in the electronic structure that can be traced by investigating the optical conductivity ($sigma(omega)$) spectra. Remarkably, the temperature variation in the $sigma(omega)$ spectrum is still present in the more localized case, even though the Kondo effect is strongly suppressed. Here, we clarify the local and itinerant character in the electronic structure by investigating the temperature dependence in the $sigma(omega)$ spectra of various Ce and Yb compounds with a tetragonal ThCr$_2$Si$_2$-type crystal structure. We explain the temperature change in a unified manner. Above temperatures of about 100 K, the temperature dependence of the $sigma(omega)$ spectra is mainly due to the electron-phonon interaction, while the temperature dependence below is due to the Kondo effect.
The rare-earth nitride ferromagnetic semiconductors owe their varying magnetic properties to the progressive filling of 4f shell across the series. Recent electrical transport measurements on samarium nitride, including the observation of superconductivity, have been understood in terms of a contribution from a 4f transport channel. Band structure calculations generally locate an empty majority 4f-band within the conduction band although over a wide range of possible energies. Here we report optical reflection and transmission measurements on samarium nitride between 0.01 eV to 4 eV, that demonstrate clearly that the 4f band forms the bottom of the conduction band. Results at the lowest energies show no free carrier absorption, indicating a semiconducting ground state, and supporting earlier conclusions based on transport measurements.
The temperature-dependent evolution pattern of 5f electrons helps to elucidate the long-standing itinerant-localized dual nature in plutonium-based compounds. In this work, we investigate the correlated electronic states of PuIn3 dependence on temperature by using a combination of the density functional theory and the dynamical mean-field theory. Not only the experimental photoemission spectroscopy is correctly reproduced, but also a possible hidden 5f itinerant-localized crossover is identified. Moreover, it is found that the quasiparticle multiplets from the many-body transitions gradually enhance with decreasing temperature, accompanied by the hybridizations with 5f electrons and conduction bands. The temperature-induced variation of Fermi surface topology suggests a possible electronic Lifshitz transition and the onset of magnetic order at low temperature. Finally, the ubiquitous existence orbital selective 5f electron correlation is also discovered in PuIn3. These illuminating results shall enrich the understanding on Pu-based compounds and serve as critical predictions for ongoing experimental research.
Ferromagnetic quantum critical points were predicted to be prohibited in clean itinerant ferromagnetic systems, yet such a phenomenon was recently revealed in CeRh$_6$Ge$_4$, where the Curie temperature can be continuously suppressed to zero under a moderate hydrostatic pressure. Here we report the observation of quantum oscillations in CeRh$_6$Ge$_4$ from measurements using the cantilever and tunnel-diode oscillator methods in fields up to 45 T, clearly demonstrating that the ferromagnetic quantum criticality occurs in a clean system. In order to map the Fermi surface of CeRh$_6$Ge$_4$, we performed angle-dependent measurements of quantum oscillations at ambient pressure, and compared the results to density functional theory calculations. The results are consistent with the Ce 4f electrons remaining localized, and not contributing to the Fermi surface, suggesting that localized ferromagnetism is a key factor for the occurrence of a ferromagnetic quantum critical point in CeRh$_6$Ge$_4$.
The CeIn3-xSnx cubic heavy fermion system presents an antiferromagnetic transition at T_N = 10 K, for x = 0, that decreases continuously down to 0 K upon Sn substitution at a critical concentration of x_c ~ 0.65. In the vicinity of T_N -> 0 the system shows non-Fermi liquid behavior due to antiferromagnetic critical fluctuations. For a high Sn content, x > 2.2, intermediate valence effects are present. In this work we show that Gd3+-doped electron spin resonance (ESR) probes a change in the character of the Ce 4f electron, as a function of Sn substitution. The Gd3+ ESR results indicate a transition of the Ce 4f spin behavior from localized to itinerant. Near the quantum critical point, on the antiferromagnetic side of the magnetic phase diagram, both localized and itinerant behaviors coexist.
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