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Orbitals and Interpretation of Photoelectron Spectroscopy Experiments and (e,2e) Ionization Experiments.

Electron momentum spectroscopy (EMS), scanning tunneling microscopy (STM), and photoelectron spectroscopy (PES) provide unique information about electronic structure, but their interpretation has been controversial. This essay discusses a framework for interpretation. Although the interpretation presented here are not new, we believe it is important to present this framework in light of recent publications. The key point is that these experiments provide information about how the electron distribution changes upon ionization, not how electrons behave in the pre-ionized state. Therefore these experiments do not lead to a "selection of the correct orbitals" in chemistry, and they do not overturn the well-known conclusion that both delocalized molecular orbitals and localized molecular orbitals are useful for interpreting chemical structure and dynamics. The two types of orbitals can produce identical total molecular electron densities and therefore molecular properties. Different types of orbitals are useful for different purposes.