铀和钚金属间化合物中5 f轨道的多组态性质
Multiconfigurational nature of 5f orbitals in uranium and plutonium intermetallics
摘要：
铀和钚的5 f电子在与配体spd态的强键结合和靠近原子核的位置之间微妙地平衡着。这些元素及其化合物的不寻常性质（例如，元素钚的六种不同同素异形体）被广泛认为取决于f-轨道占有率和离域的相关属性，但缺乏定量测量。通过采用共振X射线发射光谱（RXES）和X射线吸收近边结构（XANES）光谱和比热测量进行比较，我们证明了存在的多组态f-轨道状态的锕系元素U和Pu，并在广泛的铀和钚金属间化合物。这些结果提供了一个强大的实验基础，为理解强关联行为的锕系元素材料的新框架。
英文摘要：
Uranium and plutonium's 5f electrons are tenuously poised between strongly bonding with ligand spd-states and residing close to the nucleus. The unusual properties of these elements and their compounds (eg. the six different allotropes of elemental plutonium) are widely believed to depend on the related attributes of f-orbital occupancy and delocalization, for which a quantitative measure is lacking. By employing resonant x-ray emission spectroscopy (RXES) and x-ray absorption near-edge structure (XANES) spectroscopy and making comparisons to specific heat measurements, we demonstrate the presence of multiconfigurational f-orbital states in the actinide elements U and Pu, and in a wide range of uranium and plutonium intermetallic compounds. These results provide a robust experimental basis for a new framework for understanding the strongly-correlated behavior of actinide materials.
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