First-principles phase stability, bonding, and electronic structure of actinide metals

作者：Soederlind Per

来源：Journal of Electron Spectroscopy and Related Phenomena, 2014, 194: 2-7.

DOI：10.1016/j.elspec.2013.11.009

• Actinides
• Electronic structure
• Phase stability
• Density-functional theory

The actinide elemental metals are scare, often toxic and radio active, causing challenges for both experiments and theory while offering fascinating physics. For practical purposes they are the prevalent building blocks for materials where nuclear properties are of interest. Here, however, we are focusing on fundamental properties of the actinides related to their electronic structure and characteristic bonding in the condensed state. The series of actinides is naturally divided into two segments. First, the set of lighter actinides thorium through plutonium, often referred to as the early actinides, displays a variation of the atomic volume reminiscent of what is seen in transition metals, suggesting a gradual occupation of bonding 5f states. Second, the heavier (late) actinides, Am and onwards, demonstrate volume behaviors comparable to the rare-earth metals that implies nonbonding 5f states. Arguably, one can distinguish plutonium metal as special case lying between these two subsets because it shares some features from both. Therefore, we discuss the early actinides, plutonium metal, and the late actinides separately applying first-principles density-functional-theory (DFT) calculations. The analysis includes successes and failures of the theory to describe primarily phase stability, bonding, and electronic structure.

• 出版日期2014-6