Department of Physics, Boston College, Chestnut Hill, Massachusetts 02467, USA.
Nat Mater. 2013 Aug;12(8):707-13. doi: 10.1038/nmat3653. Epub 2013 May 26.
The Ruddlesden-Popper series of iridates (Srn+1IrnO3n+1) have been the subject of much recent attention due to the anticipation of emergent phenomena arising from the cooperative action of spin-orbit-driven band splitting and Coulomb interactions. However, an ongoing debate over the role of correlations in the formation of the charge gap and a lack of understanding of the effects of doping on the low-energy electronic structure have hindered experimental progress in realizing many of the predicted states. Using scanning tunnelling spectroscopy we map out the spatially resolved density of states in Sr3Ir2O7 (Ir327). We show that its parent compound, argued to exist only as a weakly correlated band insulator, in fact possesses a substantial ~ 130 meV charge excitation gap driven by an interplay between structure, spin-orbit coupling and correlations. We find that single-atom defects are associated with a strong electronic inhomogeneity, creating an important distinction between the intrinsic and spatially averaged electronic structure. Combined with first-principles calculations, our measurements reveal how defects at specific atomic sites transfer spectral weight from higher energies to the gap energies, providing a possible route to obtaining metallic electronic states from the parent insulating states in the iridates.
由于自旋轨道驱动能带分裂和库仑相互作用的协同作用所产生的新兴现象的预期,Ruddlesden-Popper 系列的铱酸盐(Srn+1IrnO3n+1)成为了近期研究的热点。然而,关于相关性在形成电荷间隙中的作用的持续争论,以及对掺杂对低能电子结构影响的理解不足,阻碍了实验在实现许多预测状态方面的进展。使用扫描隧道光谱学,我们描绘了 Sr3Ir2O7(Ir327)中空间分辨的态密度。我们表明,其母体化合物,被认为仅作为弱相关的带绝缘体能存在,实际上具有由结构、自旋轨道耦合和相关性相互作用驱动的实质性约 130meV 的电荷激发能隙。我们发现,单原子缺陷与强烈的电子非均匀性有关,从而在本征和空间平均电子结构之间产生了重要的区别。结合第一性原理计算,我们的测量结果揭示了特定原子位置的缺陷如何将光谱权重从高能转移到间隙能量,从而为从铱酸盐的母体绝缘态获得金属电子态提供了一种可能的途径。