Durand P, Darling G R, Dubitsky Y, Zaopo A, Rosseinsky M J
Department of Chemistry, University of Liverpool, Liverpool L69 7ZD, UK.
Nat Mater. 2003 Sep;2(9):605-10. doi: 10.1038/nmat953. Epub 2003 Aug 10.
Electron correlation controls the properties of important materials such as superconducting and magnetoresistive transition metal oxides and heavy fermion systems. The role of correlation in driving metal-to-insulator transitions assumes further importance because many superconducting materials are located close to such transitions. The nature of the insulating ground state often reveals the dominant interactions in the superconductor, as shown by the importance of the properties of La2CuO4 in understanding the high-temperature-superconducting cuprates. The A3C60 alkali metal fullerides are superconducting systems in which the role of correlation in both the normal state and the superconducting pairing mechanism is controversial, because no magnetic insulator comparable to the superconducting materials has been identified. We describe the first example of a cubic C60(3-) system with degenerate orbitals that adopts the Mott-Hubbard insulating localized electron ground state. Electron repulsion is identified as the interaction that is suppressed on the transition to metallic and superconducting behaviour in the fullerides. This observation is combined with ab initio calculations to demonstrate that it is the orbital degeneracy that allows the superconducting cubic A3C60 fullerides to remain metallic while provoking electron localization in systems with lower symmetry.
电子关联控制着重要材料的性质,如超导和磁阻过渡金属氧化物以及重费米子体系。关联在驱动金属 - 绝缘体转变中所起的作用显得尤为重要,因为许多超导材料都处于此类转变附近。绝缘基态的性质常常揭示了超导体中的主导相互作用,就像La2CuO4的性质在理解高温超导铜酸盐方面的重要性所表明的那样。A3C60碱金属富勒化物是超导体系,其中关联在正常态和超导配对机制中的作用存在争议,因为尚未发现与超导材料类似的磁绝缘体。我们描述了具有简并轨道的立方C60(3-)体系的首个例子,该体系采用莫特 - 哈伯德绝缘局域电子基态。电子排斥被确定为在富勒化物向金属态和超导态转变时被抑制的相互作用。这一观察结果与从头算相结合,以证明正是轨道简并使得超导立方A3C60富勒化物保持金属态,同时在对称性较低的体系中引发电子局域化。