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We report an experimental investigation on the irradiation of copper thinfilms with high repetition rate femtosecond laser pulses (1040 nm, 50 MHz), inambient air and liquid water. We observe a novel, striking phenomenon ofchromatic copper oxides (cupric oxide and cuprous oxide) annuli generation. Thecharacteristic features of the chromatic copper oxide annuli are studied byexploiting micro-Raman Spectroscopy, Optical and Scanning ElectronMicroscopies. In the case of irradiation in water, the seldom investigatedeffects of the immersion time, after irradiation with a fixed number of pulses,is analyzed, and an intriguing dependence of the color of the chromatic annulion the immersion time is observed. This remarkable behavior is explained byproposing an interpretation scenario addressing the various processes involvedin the process. Our experimental findings show that cuprous oxide nanoparticles(size of ~20 nm) and cuprous oxide nanocubes (nanocube edges of ~30, ~60 nm)with extremely fine sizes can be effectively generated by exploiting highrepetition rate laser-assisted oxidation.

Chromatic annuli formation and sample oxidation on copper thin films by femtosecond laser