182 research outputs found
Recommended from our members
Cancellation of spin and orbital magnetic moments in (delta)-Pu: theory
Density functional theory (DFT), in conjunction with the fixed-spin-moment (FSM) method, spin-orbit coupling (SO), and orbital polarization (OP), is shown to retain key features of the conventional DFT treatment of {delta}-Pu while at the same time not producing the substantial net magnetic moments commonly predicted by this theory. It is shown that when a small adjustment of the spin moment (less than 20%) is allowed, a complete spin- and orbital-moment cancellation occurs which results in a zero net magnetic moment in {delta}-Pu. This minor modification, accomplished by the FSM method, is shown to have a very small effect on the calculated total energy as well as the electron density-of-states (DOS). The photoemission spectra (PES), obtained from the DOS of the present model, compares equal or better to measured spectra, than that of two other recent non-magnetic models for {delta}-Pu
Recommended from our members
Phase stability in heavy f-electron metals from first-principles theory
The structural phase stability of heavy f-electron metals is studied by means of density-functional theory (DFT). These include temperature-induced transitions in plutonium metal as well as pressure-induced transitions in the trans-plutonium metals Am, Cm, Bk, and Cf. The early actinides (Th-Np) display phases that could be rather well understood from the competition of a crystal-symmetry breaking mechanism (Peierls distortion) of the 5f states and electrostatic forces, while for the trans-plutonium metals (Am-Cf) the ground-state structures are governed by 6d bonding. We show in this paper that new physics is needed to understand the phases of the actinides in the volume range of about 15-30 {angstrom}{sup 3}. At these volumes one would expect, from theoretical arguments made in the past, to encounter highly complex crystal phases due to a Peierls distortion. Here we argue that the symmetry reduction associated with spin polarization can make higher symmetry phases competitive. Taking this into account, DFT is shown to describe the well-known phase diagram of plutonium and also the recently discovered complex and intriguing high-pressure phase diagrams of Am and Cm. The theory is further applied to investigate the behaviors of Bk and Cf under compression
Recommended from our members
Quantifying the importance of orbital over spin correlations in delta-Pu within density-functional theory
Recommended from our members
Delocalization and new phase in Americium: theory
Density-functional electronic structure calculations have been used to investigate the high pressure behavior of Am. At about 80 kbar (8 GPa) calculations reveal a monoclinic phase similar to the ground state structure of plutonium ({alpha}-Pu). The experimentally suggested {alpha}-U structure is found to be substantially higher in energy. The phase transition from fcc to the low symmetry structure is shown to originate from a drastic change in the nature of the electronic structure induced by the elevated pressure. A calculated volume collapse of about 25% is associated with the transition. For the low density phase, an orbital polarization correction to the local spin density (LSD) theory was applied. Gradient terms of the electron density were included in the calculation of the exchange/correlation energy and potential, according to the generalized gradient approximation (GGA). The results are consistent with a Mott transition; the 5f electrons are delocalized and bonding on the high density side of the transition and chemically inert and non-bonding (localized) on the other. Theory compares rather well with recent experimental data which implies that electron correlation effects are reasonably modeled in our orbital polarization scheme
Recommended from our members
Quantifying the importance of orbital over spin correlations in delta-Pu within density-functional theory
Spin and orbital and electron correlations are known to be important when treating the high-temperature {delta} phase of plutonium within the framework of density-functional theory (DFT). One of the more successful attempts to model {delta}-Pu within this approach has included condensed-matter generalizations of Hund's three rules for atoms, i.e., spin polarization, orbital polarization, and spin-orbit coupling. Here they perform a quantitative analysis of these interactions relative rank for the bonding and electronic structure in {delta}-Pu within the DFT model. The result is somewhat surprising in that spin-orbit coupling and orbital polarization are far more important than spin polarization for a realistic description of {delta}-Pu. They show that these orbital correlations on their own, without any formation of magnetic spin moments, can account for the low atomic density of the {delta} phase with a reasonable equation-of-state. In addition, this unambiguously non-magnetic (NM) treatment produces a one-electron spectra with resonances close to the Fermi level consistent with experimental valence band photoemission spectra
Recommended from our members
FIRST-PRINCIPLES PHASE DIAGRAM OF THE Ce-Th SYSTEM
Actinide physics has seen a remarkable focus the last decade or so due to the combination of improved experimental diamond-anvil-cell techniques and the development of fast computers and more advanced theory. All f-electron systems are expected to have multiphase phase diagrams due to the sensitivity of the f-electron band to external influences such as pressure and temperature. For instance, compression of an f-electron metal generally causes the occupation of f-states to change due to the shift of these bands relative to others. This can in some cases, as in the Ce-Th system, cause the crystal to adopt a lower symmetry structure at elevated pressures. Here we study the phase stabilities of Ce, Th, and the Ce-Th system as a function of compression. Theoretically, both Ce and Th metals are rather well described within the DFT, although a proper treatment of the Ce-Th alloys has not yet been presented. In the present paper we revisit this problem by applying the modern theory of random alloys based on the coherent potential approximation (CPA)
Recommended from our members
Melting of Xenon to 80 GPa, p-d hybridization, and an ISRO liquid
Measurements made in a laser heated diamond-anvil cell are reported that extend the melting curve of Xe to 80 GPa and 3350 K. The steep lowering of the melting slope (dT/dP) that occurs near 17 GPa and 2750 K results from the hybridization of the p-like valence and d-like conduction states with the formation of clusters in the liquid having Icosahedral Short-Range Order (ISRO)
Recommended from our members
Atomic-volume variations of (alpha)-Pu alloyed with Al, Ga, and Am from first-principles theory
First-principles methods are employed to calculate the ground-state atomic densities (or volumes) of {alpha}-Pu alloyed with Al, Ga, and Am. Three configurations for the alloying atom are considered. (1) It is located at the most open and energetically most favorably site. (2) It is located in the least open site. (3) It is randomly distributed within the {alpha}-Pu matrix. When alloyed with Al or Ga, {alpha}-Pu behaves similarly, it expands considerably for configurations (2) and (3), while for (1) only small changes of the density occurs. Interestingly, for Am the alloying effects are quite different from that of Al and Ga. Small expansion is noted for the ordered configurations (1) and (2), whereas for the disordered (3), only insignificant changes of the density take place. The bonding character is thus differently influenced in Pu by the addition of Al and Ga on one hand and Am on the other. This is consistent with the view that Al and Ga stabilize the {delta} over the {alpha} phase in Pu by a different mechanism than Am, as has been discussed in recent publications
- …