Assessment of delocalized and localized molecular orbitals through electron momentum spectroscopy

Recently, there was a hot controversy about the concept of localized orbitals, which was triggered by Grushow's work titled "Is it time to retire the hybrid atomic orbital?" [J. Chem. Educ. 88, 860 (2011)]. To clarify the issue, we assess the delocalized and localized molecular orbitals from an experimental view using electron momentum spectroscopy. The delocalized and localized molecular orbitals based on various theoretical models for CH4, NH3, and H2O are compared with the experimental momentum distributions. Our results show that the delocalized molecular orbitals rather than the localized ones can give a direct interpretation of the experimental (e, 2e) results.