Effect of Coulomb correlations on the electronic structure of PuCoGa(5)

We investigate the effect of strong Coulomb correlations on the electronic structure of the Pu-based superconductor PuCoGa5 by employing the relativistic local spin density approximation+ Hubbard U (LSDA+U) method. The inclusion of intra-atomic Coulomb U and exchange J parameters leads to a significant reconstruction of the f states electronic structure over that given by the LSDA approach. At variance with the LSDA, the LSDA+U suggests "jj"-like coupling for the Pu 5f manifold.     

Superconductivity caused by the pairing of plutonium 5f Eelectrons in PuCoGa5

On the basis of electronic structure calculations we identify the superconductivity in the novel, high-temperature superconductor PuCoGa5 to be caused by the pairing of Pu 5f electrons. Assuming delocalized Pu 5f states, we compute theoretical crystallographic constants very near to the experimental ones, and the calculated specific heat coefficient compares reasonably to the measured coefficient. The theoretical Fermi surface is quasi-two-dimensional and the material appears to be close to a magnetic phase instability.     

非传统超导PuCoGa5晶体结构和电子性质的密度泛函理论研究

基于密度泛函理论的全势能线性缀加平面波方法（FLAPW）,采用局域自旋密度近似（LSDA）及LSDA+U方法报道了Pu基超导体系PuCoGa₅的晶格参数,原子占位和电子性质.LSDA+U方法不仅考虑Pu-5f而且考虑了Co-3d的库伦排斥作用U和Hund交换相关作用J.结果表明LSDA+U在同时考虑Pu和Co的强关联作用时晶格参数和原子占位与相关理论和实验数据吻合较好,特别是PuCoGa₅中Pu-5f的强定域特征尤其是自旋向下的电子.此外,Pu-5f与Co-3d电子的轨道杂化明显强于Ga-4p电子.     

Spin fluctuations and the peak-dip-hump feature in the photoemission spectrum of actinides

We present first-principles multiband spin susceptibility calculations within the random-phase approximation for four isostructural superconducting PuCoIn{5}, PuCoGa{5}, PuRhGa{5}, and nonsuperconducting UCoGa{5} actinides. The results show that a strong peak in the spin-fluctuation dressed self-energy is present around 0.5 eV in all materials, which is mostly created by 5f electrons. These fluctuations couple to the single-particle spectrum and give rise to a peak-dip-hump feature, characteristic of the coexistence of itinerant and localized electronic states. Results are in quantitative agreement with photoemission spectra. Finally, we show that the studied actinides can be understood within the rigid-band filling approach, in which the spin-fluctuation coupling constant follows the same materials dependence as the superconducting transition temperature T{c}.     

Pb-Pu superlattices: an example of nanostructured actinide materials

Density functional theory applied to Pb-Pu superlattices reveals two competing phases separated by a Mott transition between itinerant and localized 5f electrons. One phase, corresponding to Pu's bulk alpha phase, exhibits paired up Pu planes, thereby broadening the 5f bandwidth. Allowing spin polarization to emulate the energetics of electron correlation leads to another phase with larger volume, narrow 5f bandwidth, and more uniform local crystal structure, similar to bulk fcc Pu.     

Neutron magnetic form factor in strongly correlated materials

We introduce a formalism to compute the neutron magnetic form factor FM(q) within a first-principles density functional theory and dynamical mean field theory. The approach treats spin and orbital interactions on the same footing and reduces to earlier methods in the fully localized or the fully itinerant limit. We test the method on various actinides of current interest NpCoGa5, PuSb and PuCoGa5, and we show that PuCoGa5 is in mixed valent state, which naturally explains the measured magnetic form factor.     

Localized 5f electrons in superconducting PuCoIn?: consequences for superconductivity in PuCoGa?

The physical properties of the first In analog of the PuMGa(5) (M = Co, Rh) family of superconductors, PuCoIn(5), are reported. With its unit cell volume being 28% larger than that of PuCoGa(5), the characteristic spin-fluctuation energy scale of PuCoIn(5) is three to four times smaller than that of PuCoGa(5), which suggests that the Pu 5f electrons are in a more localized state relative to PuCoGa(5). This raises the possibility that the high superconducting transition temperature T(c) = 18.5 K of PuCoGa(5) stems from the proximity to a valence instability, while the superconductivity at T(c) = 2.5 K of PuCoIn(5) is mediated by antiferromagnetic spin fluctuations associated with a quantum critical point.     

f Electron contribution to the change of electronic structure in CeRu2Si2 with temperature: a Compton scattering study

High resolution Compton profiles have been measured in the single crystal of CeRu(2)Si(2) above and below the Kondo temperature to elucidate the change of the Ce-4f electron from localized to itinerant states. Two-dimensional electron occupation number densities projected on the first Brillouin zone, which are obtained after a series of analyses, clearly specify the difference between itinerant and localized states. The contribution of Ce-4f electrons to the electronic structure is discussed by contrast with a band calculation.     

Electronic structure and the Fermi surface of PuCoGa5 and NpCoGa5

Using a relativistic linear augmented-plane-wave method, we clarify energy band structures and Fermi surfaces of recently discovered plutonium-based superconductor PuCoGa5 and the isostructural material NpCoGa5. For PuCoGa5, we find several cylindrical sheets of Fermi surfaces with large volume, similar to CeMIn5, while for NpCoGa5, the Fermi surfaces are found to be similar to those of UMGa5. These similarities are discussed based on the j-j coupling scheme, suggesting some hints for the superconducting mechanism in HoCoGa5-type f-electron compounds.     

Spin superstructure and noncoplanar ordering in metallic pyrochlore magnets with degenerate orbitals

We study double-exchange models with itinerant t(2g) electrons in spinel and pyrochlore crystals. In both cases the localized spins form a network of corner-sharing tetrahedra. We show that the strong directional dependence of t(2g) orbitals leads to unusual Fermi surfaces that induce spin superstructures and noncoplanar orderings for a weak coupling between itinerant electrons and localized spins. Implications of our results to ZnV(2)O(4) and Cd(2)Os(2)O(7) are also discussed.     

First-principles local density approximation （LDA）＋U and generalized gradient approximation （GGA） ＋ U studies of plutonium oxides

The electronic structures and properties of PuO2 and Pu2O3 have been studied according to the first principles by using the all-electron projector-augmented-wave （PAW） method. The local density approximation （LDA）＋U and the generalized gradient approximation （GGA）＋U formalisms have been used to account for the strong on-site Coulomb repulsion among the localized Pu 5f electrons. We discuss how the properties of PuO2 and Pu2O3 are affected by choosing the values of U and exchange-correlation potential. Also, the oxidation reaction of Pu2O3, leading to the formation of PuO2, and its dependence on U and exchange-correlation potential have been studied. Our results show that by choosing an appropriate U it is possible to consistently describe structural, electronic, and thermodynamic properties of PuO2 and Pu2O3, which enable the modelling of the redox process involving Pu-based materials.     

Structural and electronic relationships between the lanthanide and actinide elements

The similarity and difference between the solid state properties of the 4f and 5f transition metals are pointed out. The heavier 5f elements show properties which have direct correspondence to the early 4f transition metals, suggesting a localized behaviour of the 5f electrons for those metals. On the other hand, the fact that Pu metal has a 30% lower volume than its neighbour heavier element, Am, suggests a tremendous difference in the properties of the 5f electrons for this element relative to the heavier actinides. This change in behaviour between Pu and Am can be viewed as a Mott transition within the 5f shell as a function of the atomic number Z. On the metallic 5f side of the Mott transition (i.e., early actinides), the elements show most unusual crystal structures, the common feature being their low symmetry. An analogous behaviour for the lanthanides is found in cerium metal under compression, where structures typical for the light actinides have been observed experimentally. A generalized phase diagram for the actinides is shown to contain features comparable to the individual phase diagram of Ce metal. The crystal structure behaviour of the lanthanides and heavier actinides is determined by the number of 5d (or 6d) electrons in the metallic state, since for these elements the f electrons are localized and nonbonding. For the earlier actinide metals electronic structure calculations - where the 5f orbitals are treated as part of the valence bands - account very well for the observed ground state crystal structures. The distorted structures can be understood as Peierls distortions away from the symmetric bcc structure and originate from strongly bonding 5f electrons occupying relatively narrow 5f states. High pressure is an extremely useful experimental tool to demonstrate the interrelationship between the lanthanides and the actinides. This revised version was published online in July 2006 with corrections to the Cover Date.     

ARPES studies of the electronic structure of LaOFe(P, As)

We report a comparison study of LaOFeP and LaOFeAs, two parent compounds of recently discovered iron-pnictide superconductors, using angle-resolved photoemission spectroscopy. Both systems exhibit some common features that are very different from well-studied cuprates. In addition, important differences have also been observed between these two ferrooxypnictides. For LaOFeP, quantitative agreement can be found between our photoemission data and the LDA band structure calculations, suggesting that a weak coupling approach based on an itinerant ground state may be more appropriate for understanding this new superconducting compound. In contrast, the agreement between LDA calculations and experiments in LaOFeAs is relatively poor, as highlighted by the unexpected Fermi surface topology around (π, π). Further investigations are required for a comprehensive understanding of the electronic structure of LaOFeAs and related compounds.     

Severe Fermi surface reconstruction at a metamagnetic transition in Ca2-xSrxRuO4 (for 0.2 <or=x<or=0.5)

We report an electrical transport study in Ca2-xSrxRuO4 single crystals at high magnetic fields (B). For x=0.2, the Hall constant Rxy decreases sharply at an anisotropic metamagnetic transition, reaching its value for Sr2RuO4 at high fields. A sharp decrease in the coefficient of the resistivity T2 term and a change in the structure of the angular magnetoresistance oscillations for B rotating in the planes confirms the reconstruction of the Fermi surface. Our observations and local-density-approximation calculations indicate a strong dependence of the Fermi surface on Ca concentration and suggest the coexistence of itinerant and localized electronic states in single layered ruthenates.     

Electronic structure, magnetism and superconductivity of layered iron compounds

The layered iron superconductors are discussed using electronic structure calculations. The four families of compounds discovered so far, including Fe (Se, Te) have closely related electronic structures. The Fermi surface consists of disconnected hole and electron cylinders and additional hole sections that depend on the specific material. This places the materials in proximity to itinerant magnetism, both due to the high density of states and due to nesting. Comparison of density functional results and experiment provides strong evidence for itinerant spin fluctuations, which are discussed in relation to superconductivity. It is proposed that the intermediate phase between the structural transition and the SDW transition in the oxy-pnictides is a nematic phase.     

重费米子超导PuMGa5(M=Co,Rh)结构、电子和热力学性质的第一性原理研究

基于第一性原理的PBEsol+U方法研究PuCoGa5和PuRhGa5的晶体结构、弹性、电子性质、声子谱以及热力学性质.PBEsol+U方法考虑Pu-5f的库伦排斥作用U和Hund交换相关作用J.计算结果表明,PuCoGa5和PuRhGa5在PBEsol+U方法下的基态性质(包括晶格参数和原子占位)与实验数据吻合较好,...     

Direct observation of dispersive Kondo resonance peaks in a heavy-fermion system

Ce 4d-4f resonant angle-resolved photoemission spectroscopy was carried out to study the electronic structure of strongly correlated Ce 4f electrons in a quasi-two-dimensional nonmagnetic heavy-fermion system CeCoGe1.2Si0.8. For the first time, dispersive coherent peaks of an f state crossing the Fermi level, the so-called Kondo resonance, are directly observed together with the hybridized conduction band. Moreover, the experimental band dispersion is quantitatively in good agreement with a simple hybridization-band picture based on the periodic Anderson model. The obtained physical quantities, i.e., coherent temperature, Kondo temperature, and mass enhancement, are comparable to the results of thermodynamic measurements. These results manifest an itinerant nature of Ce 4f electrons in heavy-fermion systems and clarify their microscopic hybridization mechanism.     

Metal-to-semimetal transition in supercooled liquid silicon

Computer simulations, using the Stillinger-Weber potential, have previously been employed to demonstrate a liquid-liquid transition in supercooled silicon near 1060 K. From calculations of electronic structure using an empirical psuedopotential, we show that silicon undergoes an associated metal to semimetal transition with a resistivity jump of roughly 1 order of magnitude. We show that the electronic states near the Fermi energy become localized in the low temperature phase, and that changes in electronic structure between the two phases arise from a change in atomic structure, and not from a change in density.     

Elusive <Emphasis Type="Italic">s-f</Emphasis> intrasite interactions and double exchange in solids: Ferromagnetic versus nonmagnetic ground state

From the theory of many-electron states in atoms, we know that there exists a strong Coulomb repulsion, which results in the electronic term structure of atoms and is responsible for Hund’s rules. By expanding the Coulomb on-site repulsion into a multipolar series, we derive this interaction and show that it is also present in solids as a correlation effect, which means that the interaction requires a multideterminant version of the Hartree-Fock method. Of particular interest is the case where this interaction couples states of localized (f) and delocalized (s) electrons. We show that the interaction is bilinear in the creation/annihilation operators for localized electrons and bilinear in the operators for conduction electrons. To study the coupling, we consider a simple model in the framework of an effective limited configuration interaction method with one localized f-electron and one itinerant s-electron per crystal site. The on-site multipole interaction between the f- and s-electrons is explicitly taken into account. It is shown that depending on the low-lying excitation spectrum imposed by the crystal electric field, the model can lead not only to ferromagnetism but also to a nonmagnetic state. The model is relevant for solids with localized and itinerant electron states.     

LSDA+U方法研究PuO2电子结构和成键特征

采用LSDA(局域自旋密度近似) U(有效库仑相关能)方法计算研究了PuO2的电子结构和成键特征。计算的平衡体积和半导体带隙分别为0.03875 nm3和0.18 eV,与实验结果符合得很好。能态密度和电子密度的分析表明PuO2并不是纯粹的离子晶体,Pu5f和O2p轨道杂化形成共价键。计算结果有助于理解PuO2晶体中Pu5f电子的关联效应。