title: Orbital density reconstruction for molecules.
abstract: 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.
authors.affiliation: Theoretical Physics IV, University of Bayreuth, D-95440 Bayreuth, Germany.
authors.forename: M
authors.initials: M
authors.lastname: Dauth
authors.forename: T
authors.initials: T
authors.lastname: Körzdörfer
authors.forename: S
authors.initials: S
authors.lastname: Kümmel
authors.forename: J
authors.initials: J
authors.lastname: Ziroff
authors.forename: M
authors.initials: M
authors.lastname: Wiessner
authors.forename: A
authors.initials: A
authors.lastname: Schöll
authors.forename: F
authors.initials: F
authors.lastname: Reinert
authors.forename: M
authors.initials: M
authors.lastname: Arita
authors.forename: K
authors.initials: K
authors.lastname: Shimada