Temperature-dependent electronic structures, atomistic modelling and the negative thermal expansion of<i>δ</i>Pu

Yin, Zhiya; Deng, Xiaoyu; Basu, Kaushik; Yin, Qian; Kotliar, Gabriel

doi:10.1080/09500839.2014.953617

Cited by 11 publications

(6 citation statements)

References 38 publications

Supporting

Mentioning

Contrasting

Unclassified

Order By: Relevance

“…It usually stabilizes under high temperature, but doping it with a few percent trivalent metal impurities (such as Ga and Al) makes it metastable at room temperature 1-3 . The δ phase has negative thermal expansion coefficient, unlike the vast majority of metallic materials [19][20][21] . The Pauli-like magnetic susceptibility, electrical resistivity, and Sommerfeld coefficient of the specific heat of δ-Pu are an order of magnitude larger than those of the other simple metals 15,17,22 .…”

Section: Introductionmentioning

confidence: 99%

Nature of the 5f electronic structure of plutonium

2020

Phys. Rev. B

View full text Add to dashboard Cite

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. Understanding 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 α, β, γ, δ, δ , and 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 α, β, and γ 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 δ phase, but also all the six allotropes are archetypal mixedvalence metals with remarkable atomic eigenstate fluctuation. In consequence of that, the 5 f occupancy n 5 f is around 5.1 ∼ 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 δ phase are the most correlated and localized.

show abstract

Section: Introductionmentioning

confidence: 99%

Nature of the 5f electronic structure of plutonium

2020

Phys. Rev. B

View full text Add to dashboard Cite

show abstract

“…In fact, above room temperature, the contributions to the free energy of the nonadiabatic effects and of the thermal excitations of the electrons from their ground state are expected to be negligible in Pu [90]. Consequently, the total energy could be used to investigate this problem either within direct Monte Carlo simulations or using molecular dynamics [101,102] with atomistic potentials extrapolated from this work.…”

Section: Phase Diagram Of Plutoniummentioning

confidence: 99%

Phase Diagram and Electronic Structure of Praseodymium and Plutonium

Lanatà¹,

Yao²,

et al. 2015

View full text Add to dashboard Cite

We develop a new implementation of the Gutzwiller approximation in combination with the local density approximation, which enables us to study complex 4f and 5f systems beyond the reach of previous approaches. We calculate from first principles the zero-temperature phase diagram and electronic structure of Pr and Pu, finding good agreement with the experiments. Our study of Pr indicates that its pressure-induced volume-collapse transition would not occur without change of lattice structure-contrarily to Ce. Our study of Pu shows that the most important effect originating the differentiation between the equilibrium densities of its allotropes is the competition between the Peierls effect and the Madelung interaction and not the dependence of the electron correlations on the lattice structure.

show abstract

“…Per the Born-Oppenheimer approximation, we assume the electrons are always in thermal equilibrium. Because strong correlations can produce a drastic suppression of the effective Fermi temperature, a strongly temperature dependent free energy functional is essential for describing correlated electronic degrees of freedom with MD [24]. In modern implementations of the GA, both the Slater determinant |Ψ 0 and the variational parameters {d i } are to be optimized through iterations [25].…”

mentioning

confidence: 99%

Mott Transition in a Metallic Liquid: Gutzwiller Molecular Dynamics Simulations

et al. 2017

View full text Add to dashboard Cite

We present a formulation of quantum molecular dynamics that includes electron correlation effects via the Gutzwiller method. Our new scheme enables the study of the dynamical behavior of atoms and molecules with strong electron interactions. The Gutzwiller approach goes beyond the conventional mean-field treatment of the intra-atomic electron repulsion and captures crucial correlation effects such as band narrowing and electron localization. We use Gutzwiller quantum molecular dynamics to investigate the Mott transition in the liquid phase of a single-band metal and uncover intriguing structural and transport properties of the atoms.

show abstract

Temperature-dependent electronic structures, atomistic modelling and the negative thermal expansion ofδPu

Cited by 11 publications

References 38 publications

Nature of the 5f electronic structure of plutonium

Nature of the 5f electronic structure of plutonium

Phase Diagram and Electronic Structure of Praseodymium and Plutonium

Mott Transition in a Metallic Liquid: Gutzwiller Molecular Dynamics Simulations

Contact Info

Product

Resources

About