The dual nature of 5f electrons and origin of heavy fermions in U compounds

We develop a theory for the electronic excitations in UPt$_3$ which is based on the localization of two of the $5f$ electrons. The remaining $f$ electron is delocalized and acquires a large effective mass by inducing intra-atomic excitations of the localized ones. The measured deHaas-vanAlphen frequencies of the heavy quasiparticles are explained as well as their anisotropic heavy mass. A model calculation for a small cluster reveals why only the largest of the different $5f$ hopping matrix elements is operative causing the electrons in other orbitals to localize.Comment: 6 pages, 3 figure

Modeling the actinides with disordered local moments

A first-principles disordered local moment (DLM) picture within the local-spin-density and coherent potential approximations (LSDA+CPA) of the actinides is presented. The parameter free theory gives an accurate description of bond lengths and bulk modulus. The case of $\delta$-Pu is studied in particular and the calculated density of states is compared to data from photo-electron spectroscopy. The relation between the DLM description, the dynamical mean field approach and spin-polarized magnetically ordered modeling is discussed.Comment: 6 pages, 4 figure

The influence of defects on magnetic properties of fcc-Pu

The influence of vacancies and interstitial atoms on magnetism in Pu has been considered in frames of the Density Functional Theory (DFT). The relaxation of crystal structure arising due to different types of defects was calculated using the molecular dynamic method with modified embedded atom model (MEAM). The LDA+U+SO (Local Density Approximation with explicit inclusion of Coulomb and spin-orbital interactions) method in matrix invariant form was applied to describe correlation effects in Pu with these types of defects. The calculations show that both vacancies and interstitials give rise to local moments in $f$-shell of Pu in good agreement with experimental data for annealed Pu. Magnetism appears due to destroying of delicate balance between spin-orbital and exchange interactions.Comment: 13 pages, 4 figure

Thermal Equation of State of Tantalum

We have investigated the thermal equation of state of tantalum from first principles using the Linearized Augmented Plane Wave (LAPW) and pseudopotential methods for pressures up to 300 GPa and temperatures up to 10000 K. The equation of state at zero temperature was computed using LAPW. For finite temperatures, mixed basis pseudopotential computations were performed for 54 atom supercells. The vibrational contributions were obtained by computing the partition function using the particle in a cell model, and the the finite temperature electronic free energy was obtained from the LAPW band structures. We discuss the behavior of thermal equation of state parameters such as the Gr\"uneisen parameter $\gamma$, $q$, the thermal expansivity $\alpha$, the Anderson-Gr\"uneisen parameter $\delta_T$ as functions of pressure and temperature. The calculated Hugoniot shows excellent agreement with shock-wave experiments. An electronic topological transition was found at approximately 200 GPa

Structure and Dynamics of Liquid Iron under Earth's Core Conditions

First-principles molecular dynamics simulations based on density-functional theory and the projector augmented wave (PAW) technique have been used to study the structural and dynamical properties of liquid iron under Earth's core conditions. As evidence for the accuracy of the techniques, we present PAW results for a range of solid-state properties of low- and high-pressure iron, and compare them with experimental values and the results of other first-principles calculations. In the liquid-state simulations, we address particular effort to the study of finite-size effects, Brillouin-zone sampling and other sources of technical error. Results for the radial distribution function, the diffusion coefficient and the shear viscosity are presented for a wide range of thermodynamic states relevant to the Earth's core. Throughout this range, liquid iron is a close-packed simple liquid with a diffusion coefficient and viscosity similar to those of typical simple liquids under ambient conditions.Comment: 13 pages, 8 figure

Iron under Earth's core conditions: Liquid-state thermodynamics and high-pressure melting curve

{\em Ab initio} techniques based on density functional theory in the projector-augmented-wave implementation are used to calculate the free energy and a range of other thermodynamic properties of liquid iron at high pressures and temperatures relevant to the Earth's core. The {\em ab initio} free energy is obtained by using thermodynamic integration to calculate the change of free energy on going from a simple reference system to the {\em ab initio} system, with thermal averages computed by {\em ab initio} molecular dynamics simulation. The reference system consists of the inverse-power pair-potential model used in previous work. The liquid-state free energy is combined with the free energy of hexagonal close packed Fe calculated earlier using identical {\em ab initio} techniques to obtain the melting curve and volume and entropy of melting. Comparisons of the calculated melting properties with experimental measurement and with other recent {\em ab initio} predictions are presented. Experiment-theory comparisons are also presented for the pressures at which the solid and liquid Hugoniot curves cross the melting line, and the sound speed and Gr\"{u}neisen parameter along the Hugoniot. Additional comparisons are made with a commonly used equation of state for high-pressure/high-temperature Fe based on experimental data.Comment: 16 pages including 6 figures and 5 table

High Pressure Thermoelasticity of Body-centered Cubic Tantalum

We have investigated the thermoelasticity of body-centered cubic (bcc) tantalum from first principles by using the linearized augmented plane wave (LAPW) and mixed--basis pseudopotential methods for pressures up to 400 GPa and temperatures up to 10000 K. Electronic excitation contributions to the free energy were included from the band structures, and phonon contributions were included using the particle-in-a-cell (PIC) model. The computed elastic constants agree well with available ultrasonic and diamond anvil cell data at low pressures, and shock data at high pressures. The shear modulus $c_{44}$ and the anisotropy change behavior with increasing pressure around 150 GPa because of an electronic topological transition. We find that the main contribution of temperature to the elastic constants is from the thermal expansivity. The PIC model in conjunction with fast self-consistent techniques is shown to be a tractable approach to studying thermoelasticity.Comment: To be appear in Physical Review