Theoretical Division, Los Alamos National Laboratory, Los Alamos, New Mexico 87545, USA.
Nat Commun. 2013;4:2644. doi: 10.1038/ncomms3644.
An understanding of the phase diagram of elemental plutonium (Pu) must include both, the effects of the strong directional bonding and the high density of states of the Pu 5f electrons, as well as how that bonding weakens under the influence of strong electronic correlations. Here we present electronic-structure calculations of the full 16-atom per unit cell α-phase structure within the framework of density functional theory together with dynamical mean-field theory. Our calculations demonstrate that Pu atoms sitting on different sites within the α-Pu crystal structure have a strongly varying site dependence of the localization-delocalization correlation effects of their 5f electrons and a corresponding effect on the bonding and electronic properties of this complicated metal. In short, α-Pu has the capacity to simultaneously have multiple degrees of electron localization/delocalization of Pu 5f electrons within a pure single-element material.
理解元素钚（Pu）的相图必须同时考虑强定向键合和 Pu 5f 电子的高密度态的影响，以及在强电子相关作用下该键合如何减弱。在这里，我们在密度泛函理论和动态平均场理论的框架内，对每个晶胞包含 16 个原子的完整 α 相结构进行了电子结构计算。我们的计算表明，位于 α-Pu 晶体结构不同位置的 Pu 原子，其 5f 电子的局域-离域相关效应的局域化程度具有强烈的位置依赖性，以及对这种复杂金属的键合和电子性质的相应影响。简而言之，在纯单相材料中，α-Pu 具有同时使 Pu 5f 电子实现多个程度的电子局域/离域的能力。
