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Unveiling the Valence Fluctuations in δ-Pu by means of High-Energy Inelastic Neutron Spectroscopy

机译:通过高能无弹性中子谱揭示Δ-PU中的价波动

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Pu is arguably the most complex elemental metal known because its 5 f electrons are tenuously poised at the edge between localized and itinerant configurations. This complex electronic structure leads to emergent behavior-all a direct consequence of its 5f electrons-including six allotropic phases, large volumetric changes associated with these transitions of up to 25%, and mechanical properties ranging from brittle δ-Pu to ductile δ-Pu. Pu also exhibits a Pauli-like magnetic susceptibility, electrical resistivity and a Sommerfeld coefficient of the specific heat that are an order of magnitude larger than in any other elemental metal. Finally, while experiments find no sign for static magnetism in Pu, most theories that use the correct volume predict a magnetically ordered state. This discrepancy might be reconciled by recent Dynamical Mean Field Theory (DMFT) calculations that indicate that the electronic configuration of δ-Pu is a quantum mechanical mixture of the fully localized 5f~5 (Pu~(3+)) and the 5f~ 6 (Pu~(2+)) configuration, resulting in a predicted valence in the range v = 5.2 - 5.4 confirmed by recent resonance x-ray emission spectroscopy experiments. The characteristic energy scale for the associated spin fluctuations is expected to be T_K = 800 K (≈ 70 meV) that will result in a dynamical spectral response centered at this energy for T < T_K.
机译:PU可以说是已知的最复杂的元素金属,因为它的5 f电子在局部和腾注配置之间的边缘处是浓度的。这种复杂的电子结构导致紧急行为 - 其5F电子的所有直接后果 - 包括六个同种异性相,与这些过渡相关的大容量变化,高达25%,以及从脆性Δ-pu到延展性Δ-pu的机械性能。 。 PU还表现出pauli样磁磁性敏感性,电阻率和躯体菲尔德系数的特定热量,其比任何其他元素金属大的数量级大。最后,虽然实验发现PU中的静态磁性没有迹象,但是使用正确体积的大多数理论都预测了磁性有序状态。该差异可能是由最近的动态平均场理论(DMFT)计算的调整,表明Δ-PU的电子配置是完全定位5F〜5(PU〜(3+))和5F〜6的量子机械混合物(PU〜(2+))配置,由最近的共振X射线发射光谱实验进行了v = 5.2 - 5.4的v = 5.2-5.4的预测性。相关旋转波动的特性能量尺度预计为T_K = 800 k(≈00mev),其将导致在该能量上以T

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