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Excimer laser irradiation of iron in air or nitrogen gas at ambient pressure was found to result in a remarkable nitriding of the surface. Nitrogen concentrations of about 12 at.% were achieved in surface layers exceeding 500 nm in depth. The formation of oxides during irradiation in air was limited to the first 100 nm of the sample. The nitrogen resulted in the formation of Fe-N austenite and ε-iron nitride in the laser-nitrided surface layer as proven by Mossbauer spectroscopy. A combination of several nuclear methods is well suited for the investigation of this process.