Plutonium-based compounds establish an ideal platform for exploring the interplay between long-standing itinerant-localized 5$f$ states and strongly correlated electronic states. In this paper, we exhaustively investigate the correlated 5$f$ electron
ic states of PuSn$_3$ dependence on temperature by means of a combination of the density functional theory and the embedded dynamical mean-field theory. It is found that the spectral weight of narrow 5$f$ band grows significantly and remarkable quasiparticle multiplets appear around the Fermi level at low temperature. A striking $c-f$ hybridization and prominent valence state fluctuations indicate the advent of coherence and itinerancy of 5$f$ states. It is predicted that a 5$f$ localized to itinerant crossover is induced by temperature accompanied by the change in Fermi surface topology. Therefore itinerant 5$f$ states are inclined to take in active chemical bonding, suppressing the formation of local magnetic moment of Pu atoms, which partly elucidates the intrinsic feature of paramagnetic ground state of PuSn$_3$. Furthermore, the 5$f$ electronic correlations are orbital selective manifested themselves in differentiated band renormalizations and electron effective masses. Consequently, the convincing results remain crucial to our understanding of plutonium-based compounds and promote ongoing research.
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 temper
ature 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.
The physical properties of plutonium and plutonium-based intermetallic compounds are extremely sensitive to temperature, pressure, and chemical alloying. A celebrated example is the high-temperature $delta$ phase plutonium, which can be stabilized at
room temperature by doping it with a few percent trivalent metal impurities, such as gallium or aluminum. The cubic phase Pu$_{3}$Ga, one of the plutonium-gallium intermetallic compounds, plays a key role in understanding the phase stability and phase transformation of the plutonium-gallium system. Its electronic structure might be essential to figure out the underlying mechanism that stabilizes the $delta$ phase plutonium-gallium alloy. In the present work, we studied the temperature-dependent correlated electronic states of cubic phase Pu$_{3}$Ga by means of a combination of the density functional theory and the embedded dynamical mean-field theory. We identified orbital selective 5$f$ itinerant-localized (coherent-incoherent) crossovers which could occur upon temperature. Actually, there exist two well-separated electronic coherent temperatures. The higher one is for the $5f_{5/2}$ state [$T_{text{coh}}(5f_{5/2}) approx 700$ K], while the lower one is for the $5f_{7/2}$ state [$T_{text{coh}}(5f_{7/2}) approx 100$ K]. In addition, the quasiparticle multiples which originate from the many-body transitions among the $5f^{4}$, $5f^{5}$, and $5f^{6}$ electronic configurations, decay gradually. The hybridizations between the localized 5$f$ bands and conduction bands are subdued by high temperature. Consequently, the Fermi surface topology is changed, which signals a temperature-driven electronic Lifshitz transition. Finally, the calculated linear specific heat coefficient $gamma$ is approximately 112 mJ / (mol K$^2$) at $T = 80$ K.
Hexagonal CoSn is a newly-discovered frustrated kagome metal. It shows close-to-textbook flat bands and orbital-selective Dirac fermions, which are largely associated with its strongly correlated Co-3$d$ orbitals. Because correlated electronic states
are easily regulated by external conditions (such as chemical doping, pressure, and temperature), the fate of these kagome-derived electronic bands upon temperature becomes an interesting and unsolved question. In this work, we try to study the temperature-dependent electronic structures of hexagonal CoSn by means of the density functional theory in conjunction with the embedded dynamical mean-field theory. We find that hexagonal CoSn is in close proximity to a Mott insulating state at ambient condition. Special attention is devoted to the evolution of its Co-3$d$ electronic states with respect to temperature. At least six different temperatures (or energy scales), namely $T^{*}$, $T_{text{FL}}$, $T_{text{S1}}$ (and $T_{text{S2}}$), $T_{text{SF}}$, and $bar{T}$, are figured out. They are related to stabilization of the pseudogap state, emergence of the non-Fermi-liquid phase, onset (and completeness) of the intermediate spin state, occurrence of the spin-frozen phase, beginning of the orbital freezing transition, respectively.
Ce$_{3}$Al is an archetypal heavy-fermion compound with multiple crystalline phases. Here, we try to investigate its electronic structures in the hexagonal phase ($alpha$-Ce$_{3}$Al) and cubic phase ($beta$-Ce$_{3}$Al) by means of a combination of de
nsity functional theory and single-site dynamical mean-field theory. We confirm that the 4$f$ valence electrons in both phases are itinerant, accompanied with strong valence state fluctuations. Their 4$f$ band structures are heavily renormalized by electronic correlations, resulting in large effective electron masses. The Kondo screening in Ce$_{3}$Al would be protracted over a wide range of temperature since the single-impurity Kondo temperature $T_{K}$ is much higher than the coherent Kondo temperature $T^{*}_{K}$. Especially, the crystal structure of $alpha$-Ce$_{3}$Al forms a layered kagome lattice. We observe conspicuous kagome-derived flat bands and Dirac cones (or gaps) in its quasiparticle band structure. Therefore, it is concluded that the hexagonal phase of Ce$_{3}$Al will be a promising candidate of heavy-fermion kagome metal.
By means of the density functional theory in combination with the dynamical mean-field theory, we tried to examine the electronic structure of hexagonal FeGe, in which the Fe atoms form a quasi-2D layered Kagome lattice. We predict that it is a repre
sentative Kagome metal characterized by orbital selective Dirac fermions and extremely flat bands. Furthermore, Fes 3$d$ electrons are strongly correlated. They exhibit quite apparent signatures of electronic correlation induced by Hunds rule coupling, such as sizable differentiation in band renormalization, non-Fermi-liquid behavior, spin-freezing state, and spin-orbital separation. Thus, FeGe can be regarded as an ideal platform to study the interplay of Kagome physics and Hundness. 5
The ground state electronic structure and magnetic behaviors of curium dioxide (CmO$_{2}$) are controversial. In general, the formal valence of Cm ions in CmO$_{2}$ should be tetravalent. It implies a $5f^{6.0}$ electronic configuration and a non-mag
netic ground state. However, it is in sharp contrast with the large magnetic moment measured by painstaking experiments. In order to clarify this contradiction, we tried to study the ground state electronic structure of CmO$_{2}$ by means of a combination of density functional theory and dynamical mean-field theory. We find that CmO$_{2}$ is a wide-gap charge transfer insulator with strong 5$f$ valence state fluctuation. It belongs to a mixed-valence compound indeed. The predominant electronic configurations for Cm ions are $5f^{6.0}$ and $5f^{7.0}$. The resulting magnetic moment agrees quite well with the experimental value. Therefore, the magnetic puzzle in CmO$_{2}$ can be appropriately explained by the mixed-valence scenario.
A combination of the density functional theory and the single-site dynamical mean-field theory is employed to study the electronic structures of various allotropes of elemental curium (Cm-I, Cm-II, and Cm-III). We find that the 5$f$ valence electrons
in the high-symmetry Cm-I and Cm-II phases remain localized, while they turn into itinerancy in the low-symmetry monoclinic Cm-III phase. In addition, conspicuous quasiparticle multiplets are identified in the 5$f$ electronic density of states of the Cm-III phase. We believe that it is the many-body transition between $5f^{7}$ and $5f^{8}$ configurations that gives rise to these quasiparticle multiplets. Therefore, the Cm-III phase is probably a new realization of the so-called Racah metal.
To unravel the interplay between the strong electronic correlation and itinerant-localized dual nature in atypical f electron systems, we employed the density functional theory in combination with the single-site dynamical mean-field theory to system
atically investigate the electronic structures of CeSb and USb. We find that the 4f states in CeSb are mostly localized which show a weak quasi-particle resonance peak near the Fermi level. Conversely, the 5f electrons in USb display partially itinerant feature, accompanied by mixed-valence behavior and prominent valence state fluctuations. Particularly, the 4f electronic correlations in CeSb are distinctly orbital-selective with strikingly renormalized 4f5/2 states, according to the low-energy behaviors of 4f self-energy functions. It is believed that the strong electronic correlation and fantastic bonding of f states contribute to elucidate the fascinating magnetism.
Plutonium (Pu), in which the 5$f$ valence electrons always wander the boundary between localized and itinerant states, exhibits quite complex crystal structures and unprecedentedly anomalous properties with respect to temperature and alloying. Unders
tanding its chemical and physical properties, especially its 5$f$ electronic structure is one of the central and unsolved topics in condensed matter theory. In the present work, the electronic structures of the six allotropes of Pu (including its $alpha$, $beta$, $gamma$, $delta$, $delta$, and $epsilon$ phases) at ambient pressure are studied comprehensively by means of the density functional theory in combination with the single-site dynamical mean-field theory. The band structures, total and partial density of states, valence state histograms, 5$f$ orbital occupancies, X-ray branching ratios, and self-energy functions are carefully studied. It is suggested that the $alpha$, $beta$, and $gamma$ phases of Pu are typical Racah metals in which the atomic multiple effect dominates near the Fermi level. The calculated results reveal that not only the $delta$ phase, but also all the six allotropes are archetypal mixed-valence metals with remarkable atomic eigenstate fluctuation. In consequence of that, the 5$f$ occupancy $n_{5f}$ is around 5.1 $sim$ 5.4, which varies with respect to the atomic volume and electronic correlation strength of Pu. The 5$f$ electronic correlation in Pu is moderately orbital-dependent. Moreover, the 5$f$ electrons in the $delta$ phase are the most correlated and localized.
