The vibrational properties of interstitial silane (SiH 4) i and silyl (SiH 3) i molecules in crystalline silicon are calculated using a first-principle, cluster based, spin-polarised local-density method. The Si-H stretch modes are found to be red-shifted by ∼ 300 cm −1 from those of the isolated molecule which lie around 2200 cm −1. These results refute recent suggestions that modes observed around 2200 cm −1 , and previously assigned to hydrogenated vacancy defects, are due to these interstitial molecules.