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The laser-based method for removal of sulfur (DMDBT) in hydrocarbon fuels provides for deep desulfurization of hydrogen fuels through the elimination of dimethyldibenzothiophene (DMDBT) from hydrocarbon fuels. The method involves photoexciting atomic or molecular oxygen to a singlet or triplet energy state, mixing the photoexcited oxygen with the hydrocarbon fuel, and irradiating the hydrocarbon fuel with UV radiation from a tunable laser source at a wavelength corresponding to an absorption band of dimethyldibenzothiophene. The hydrocarbon fuel may be in a liquid or an aerosol state. The oxygen may be provided by pure oxygen gas, by N2O, or by air, and may be diluted by an inert carrier gas, such as N2. Exemplary wavelengths of the laser radiation include 193 nm, 248 nm, and 266 nm. Sulfur is eliminated from DMDBT as elemental sulfur or gaseous sulfides and sulfur oxides, which are easily separated from the hydrocarbon fuels.