Isotopes of a gaseous compound can be separated by multi-infrared photoabsorption which follows a selective dissociation of the excited molecules by single photon absorption of photons of visible or UV radiation. The process involves three steps. Firstly, the molecules to be separated are irradiated with a high-energy IR laser, whereby the molecules of the compound containing the lighter isotopes are preferably excited. They are then irradiated by a second laser with UV or visible light whose frequency of radiation brings the excited molecules into a form in which they can be separated from the non-excited molecules. The third step is the reformation of the substances according to known methods. A power density of at least 10/sup 4/ watt/cm/sup 2/ per torr gas pressure with an irradiation time of 10/sup -10/ to 5 x 10/sup -5/ seconds in the presence of a second gas with at least 5 times higher partial pressure is necessary for the IR radiation. The method may be used for UF/sub 6/ for which an example is given here.