Institute for Solid State Physics, The University of Tokyo, Kashiwa, Chiba 277-8581, Japan.
J Phys Condens Matter. 2010 Mar 10;22(9):095502. doi: 10.1088/0953-8984/22/9/095502. Epub 2010 Feb 10.
CeOs(4)Sb(12) and CeFe(4)P(12) are classified as Kondo semiconductors, which show coupled changes in electrical transport, thermodynamic and magnetic properties with a low-temperature semiconductor-like electrical resistivity. We have carried out core level and valence band photoemission spectroscopy on single crystal CeOs(4)Sb(12) and CeFe(4)P(12) to study their electronic structure and the evolution of states at the Fermi level as a function of temperature (∼10-300 K). The Ce 3d core level spectra show the presence of f(0), f(1) and f(2) final states with very different relative intensities in the two compounds. Single-impurity Anderson model calculations provide f electron counts of n(f) = 0.97 and 0.86 per Ce atom, suggestive of a low- and high-T(K) (= single ion Kondo temperature) for CeOs(4)Sb(12) and CeFe(4)P(12), respectively. The high-resolution temperature-dependent near-Fermi level spectra show pseudogaps of energy ∼ 50 meV and ∼ 110 meV in the valence band density of states (DOS) of CeOs(4)Sb(12) and CeFe(4)P(12), respectively. The temperature dependence of the DOS at the Fermi level follows the change in effective magnetic moment estimated from magnetic susceptibility for both materials, confirming the Kondo nature of the pseudogap in CeOs(4)Sb(12) and CeFe(4)P(12). A compilation of measured pseudogaps using photoemission and optical spectroscopy identifies the charge gaps Δ(C) for Ce-based Kondo semiconductors and provides a direct relation with T(K) given by Δ(C) ∼ 2k(B)T(K). In conjunction with the known behaviour of the spin gaps Δ(S) ∼ k(B)T(K), the results establish the coupled energy scaling of the spin and charge gaps in Kondo semiconductors.
CeOs(4)Sb(12) 和 CeFe(4)P(12) 被归类为康登半导体,它们的电输运、热力学和磁性能表现出低温半导体电阻率的耦合变化。我们对单晶 CeOs(4)Sb(12) 和 CeFe(4)P(12) 进行了芯能级和价带光电子能谱研究,以研究它们的电子结构和费米能级附近态的温度依赖性(约 10-300 K)演化。Ce 3d 芯能级谱显示出两种化合物中存在 f(0)、f(1) 和 f(2) 终态,其相对强度非常不同。单杂质安德森模型计算提供了每个 Ce 原子的 f 电子计数 n(f) = 0.97 和 0.86,分别表明 CeOs(4)Sb(12) 和 CeFe(4)P(12) 的低和高 T(K)(=单离子康登温度)。高分辨率温度依赖近费米能级谱显示 CeOs(4)Sb(12) 和 CeFe(4)P(12) 的价带态密度(DOS)中能量约为 50 meV 和 110 meV 的赝隙。费米能级附近 DOS 的温度依赖性与两种材料的磁磁化率估计的有效磁矩变化一致,证实了 CeOs(4)Sb(12) 和 CeFe(4)P(12) 中赝隙的康登性质。使用光电子能谱和光学光谱测量的赝隙汇总确定了 Ce 基康登半导体的电荷间隙 Δ(C),并给出了由 Δ(C)∼2k(B)T(K) 给出的 T(K)的直接关系。结合已知的自旋间隙 Δ(S)∼k(B)T(K) 的行为,结果确立了康登半导体中自旋和电荷间隙的耦合能量标度。