We have developed an all-electron density-functional (AE-DF) program using
the Mexican hat wavelet. The AE-DF program is applied to the ab initio all-
electron calculations of small molecules as prototype systems, and the cons
truction scheme of multiresolution support spheres is used to optimize the
computational efficiency. Convergences are systematically demonstrated as a
function of the number of resolution levels and support sphere sizes. Deta
iled analyses of H-2, CO, and H2O molecules and the Is core-ionized C*O and
CO* molecules show good agreement with experiments and other theoretical w
orks. The results indicate that one can gain computational efficiency by se
veral orders of magnitude over the plane-wave-based methods in these molecu
les. [S0163-1829(99)00827-9].