This paper discusses the physical principles involved in creating a fullerene-oxygen-iodine laser (FOIL) with optical (including solar) pumping. The kinetic layout is discussed, and it is shown that the limiting efficiency of a FOIL can exceed 40% relative to the energy absorbed by the fullerenes. Experimental results of the lasing of singlet oxygen in liquid media (solutions and suspensions) and in solid-state structures containing both fullerenes and fullerenelike nanoparticles (FLNs) are presented. It is experimentally shown to be possible to release oxygen in the vapor phase by organizing the boiling of a solution (suspension), as well as by a gasdynamic desorption wave from solid-state FLN- or fullerene-containing structures. Preliminary experimental results are presented of the pulsed lasing of a FOIL with optical pumping, using the initial photodissociation of iodide to provide atomic iodine in the lasing zone. The principle of spectral separation of optical pumping is implemented in experiments on the lasing of a FOIL.

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