Abstract
A method is described for the calculation of momentum distributions and Compton profiles of polyatomic molecules. Distributions, profiles and momentum expectation values are calculated for the boron hydrides B2H6, B4H10, B5H9, B5H11, and B6H10. Contour maps of total and difference densities in momentum space are presented for diborane. The results are analyzed in terms of localized orbitals. The analysis shows that traditional concepts of two‐ and three‐center electron pair bonds may find great utility in interpreting momentum space distributions.