New Pseudo-Phase Structure for α\alpha-Pu

In this paper we propose a new pseudo-phase crystal structure, based on an orthorhombic distortion of the diamond structure, for the ground-state $\alpha$-phase of plutonium. Electronic-structure calculations in the generalized-gradient approximation give approximately the same total energy for the two structures. Interestingly, our new pseudo-phase structure is the same as the Pu $\gamma$-phase structure except with very different b/a and c/a ratios. We show how the contraction relative to the $\gamma$ phase, principally in the $z$ direction, leads to an $\alpha$-like structure in the [0,1,1] plane. This is an important link between two complex structures of plutonium and opens new possibilities for exploring the very rich phase diagram of Pu through theoretical calculations

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 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

Phylogenetic relatedness and host plant growth form influence gene expression of the polyphagous comma butterfly (Polygonia c-album)

<p>Abstract</p> <p>Background</p> <p>The mechanisms that shape the host plant range of herbivorous insect are to date not well understood but knowledge of these mechanisms and the selective forces that influence them can expand our understanding of the larger ecological interaction. Nevertheless, it is well established that chemical defenses of plants influence the host range of herbivorous insects. While host plant chemistry is influenced by phylogeny, also the growth forms of plants appear to influence the plant defense strategies as first postulated by Feeny (the "plant apparency" hypothesis). In the present study we aim to investigate the molecular basis of the diverse host plant range of the comma butterfly (<it>Polygonia c-album</it>) by testing differential gene expression in the caterpillars on three host plants that are either closely related or share the same growth form.</p> <p>Results</p> <p>In total 120 genes were identified to be differentially expressed in <it>P. c-album </it>after feeding on different host plants, 55 of them in the midgut and 65 in the restbody of the caterpillars. Expression patterns could be confirmed with an independent method for 14 of 27 tested genes. Pairwise similarities in upregulation in the midgut of the caterpillars were higher between plants that shared either growth form or were phylogenetically related. No known detoxifying enzymes were found to be differently regulated in the midgut after feeding on different host plants.</p> <p>Conclusion</p> <p>Our data suggest a complex picture of gene expression in response to host plant feeding. While each plant requires a unique gene regulation in the caterpillar, both phylogenetic relatedness and host plant growth form appear to influence the expression profile of the polyphagous comma butterfly, in agreement with phylogenetic studies of host plant utilization in butterflies.</p

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

A Full-Potential-Linearized-Augmented-Plane-Wave Electronic Structure Study of delta-Plutonium and the (001) Surface

The electronic and geometric properties of bulk fcc delta-plutonium and the quantum size effects in the surface energies and the work functions of the (001) ultra thin films (UTF) up to 7 layers have been investigated with periodic density functional theory calculations within the full-potential linearized augmented-plane wave (FP-LAPW) approach as implemented in the WIEN2k package. Our calculated equilibrium atomic volume of 178.3 a.u.^3 and bulk modulus of 24.9 GPa at the fully relativistic level of theory, i.e. spin-polarization and spin-orbit coupling included, are in good agreement with the experimental values of 168.2 a.u.^3 and 25 GPa (593 K), respectively. The calculated equilibrium lattice constants at different levels of approximation are used in the surface properties calculations for the thin films. The surface energy is found to be rapidly converged with the semi-infinite surface energy predicted to be 0.692eV at the fully-relativistic level.Comment: 27 pages,8 figure

Thermodynamic stability of Fe/O solid solution at inner-core conditions

We present a new technique which allows the fully {\em ab initio} calculation of the chemical potential of a substitutional impurity in a high-temperature crystal, including harmonic and anharmonic lattice vibrations. The technique uses the combination of thermodynamic integration and reference models developed recently for the {\em ab initio} calculation of the free energy of liquids and anharmonic solids. We apply the technique to the case of the substitutional oxygen impurity in h.c.p. iron under Earth's core conditions, which earlier static {\em ab initio} calculations indicated to be thermodynamically very unstable. Our results show that entropic effects arising from the large vibrational amplitude of the oxygen impurity give a major reduction of the oxygen chemical potential, so that oxygen dissolved in h.c.p. iron may be stabilised at concentrations up a few mol % under core conditions

A density functional study of molecular oxygen adsorption and reaction barrier on Pu (100) surface

Oxygen molecule adsorptions on a Pu (100) surface have been studied in detail, using the generalized gradient approximation to density functional theory. Dissociative adsorption with a layer by layer alternate spin arrangement of the plutonium layer is found to be energetically more favorable compared to molecular adsorption. Hor2 approach on a bridge site without spin polarization was found to the highest chemisorbed site with energy of 8.787 eV among all the cases studied. The second highest chemisorption energy of 8.236 eV, is the spin-polarized Hor2 or Ver approach at center site. Inclusion of spin polarization affects the chemisorption processes significantly, non-spin-polarized chemisorption energies being typically higher than the spin-polarized energies. We also find that the 5f electrons to be more localized in spin-polarized cases compared to the non-spin-polarized counterparts. The ionic part of O-Pu bonding plays a significant role, while the Pu 5f-O 2p hybridization was found to be rather week. Also, adsorptions of oxygen push the top of 5f band deeper away from the Fermi level, indicating further bonding by the 5f orbitals might be less probable. Except for the interstitial sites, the work functions increase due to adsorptions of oxygen