Theoretical Physics IV, University of Bayreuth, D-95440 Bayreuth, Germany.
Phys Rev Lett. 2011 Nov 4;107(19):193002. doi: 10.1103/PhysRevLett.107.193002.
The experimental imaging of electronic orbitals has allowed one to gain a fascinating picture of quantum effects. We here show that the energetically high-lying orbitals that are accessible to experimental visualization in general differ, depending on which approach is used to calculate the orbitals. Therefore, orbital imaging faces the fundamental question of which orbitals are the ones that are visualized. Combining angular-resolved photoemission experiments with first-principles calculations, we show that the orbitals from self-interaction-free Kohn-Sham density functional theory are the ones best suited for the orbital-based interpretation of photoemission.
电子轨道的实验成像使得人们能够获得令人着迷的量子效应图像。在这里，我们表明，一般来说，在实验中可以可视化的高能轨道根据所使用的计算轨道的方法而有所不同。因此，轨道成象面临着一个基本问题，即哪些轨道是被可视化的轨道。通过角分辨光电子发射实验与第一性原理计算的结合，我们表明，自相互作用自由的 Kohn-Sham 密度泛函理论的轨道是最适合基于轨道的光电子发射解释的轨道。
