Department of Physics, Sapienza University of Rome, Roma, Italy.
Proc Natl Acad Sci U S A. 2012 Sep 25;109(39):15685-90. doi: 10.1073/pnas.1208492109. Epub 2012 Sep 7.
Electronic functionalities in materials from silicon to transition metal oxides are, to a large extent, controlled by defects and their relative arrangement. Outstanding examples are the oxides of copper, where defect order is correlated with their high superconducting transition temperatures. The oxygen defect order can be highly inhomogeneous, even in optimal superconducting samples, which raises the question of the nature of the sample regions where the order does not exist but which nonetheless form the "glue" binding the ordered regions together. Here we use scanning X-ray microdiffraction (with a beam 300 nm in diameter) to show that for La(2)CuO(4+y), the glue regions contain incommensurate modulated local lattice distortions, whose spatial extent is most pronounced for the best superconducting samples. For an underdoped single crystal with mobile oxygen interstitials in the spacer La(2)O(2+y) layers intercalated between the CuO(2) layers, the incommensurate modulated local lattice distortions form droplets anticorrelated with the ordered oxygen interstitials, and whose spatial extent is most pronounced for the best superconducting samples. In this simplest of high temperature superconductors, there are therefore not one, but two networks of ordered defects which can be tuned to achieve optimal superconductivity. For a given stoichiometry, the highest transition temperature is obtained when both the ordered oxygen and lattice defects form fractal patterns, as opposed to appearing in isolated spots. We speculate that the relationship between material complexity and superconducting transition temperature T(c) is actually underpinned by a fundamental relation between T(c) and the distribution of ordered defect networks supported by the materials.
材料中的电子功能,从硅到过渡金属氧化物,在很大程度上受到缺陷及其相对排列的控制。铜的氧化物就是一个突出的例子,其中缺陷的有序性与它们的高温超导转变温度有关。氧缺陷的有序性可能高度不均匀,即使在最佳超导样品中也是如此,这就提出了一个问题,即不存在有序性的样品区域的性质是什么,但这些区域形成了将有序区域结合在一起的“粘结剂”。在这里,我们使用扫描 X 射线微衍射(束斑直径 300nm)来表明,对于 La(2)CuO(4+y),粘结剂区域包含非调幅局部晶格畸变,在最佳超导样品中,其空间范围最为明显。对于一个掺杂不足的单晶,其中在 CuO(2)层之间插入的 La(2)O(2+y)层中的间隙氧离子是可移动的,非调幅局部晶格畸变形成与有序氧离子反相关的液滴,在最佳超导样品中,其空间范围最为明显。在这个最简单的高温超导体中,因此存在两个有序缺陷网络,而不是一个,它们可以被调谐以实现最佳超导性。对于给定的化学计量比,当有序氧和晶格缺陷都形成分形图案时,而不是出现在孤立的点上,会获得最高的转变温度。我们推测,材料复杂性和超导转变温度 T(c)之间的关系实际上是由材料所支持的有序缺陷网络分布与 T(c)之间的基本关系所支撑的。