Orbital density reconstruction for molecules

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...

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Bibliographic Details
Published in:Physical review letters 2011-11, Vol.107 (19), p.193002-193002
Main Authors: Dauth, M, Körzdörfer, T, Kümmel, S, Ziroff, J, Wiessner, M, Schöll, A, Reinert, F, Arita, M, Shimada, K
Format: Article
Language:English
Online Access:Get full text
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Summary: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.
ISSN:1079-7114
DOI:10.1103/PhysRevLett.107.193002