UV femtosecond single-pulse and collinear double-pulse laser-induced breakdown spectroscopy (LIBS) for depth-resolved characterization of nano-scaled films

In the current work, we demonstrate the UV femtosecond (248 nm, 450 fs) single-pulse and double-pulse laser-induced breakdown spectroscopy (LIBS) as an effective method for depth profiling of nanometer-thick multi-layered structures, including photovoltaic thin films. Femtosecond LIBS enabled selective detection of both organic and inorganic materials at different depths within nanometer-scale (10–250 nm) multi-layered samples having thicknesses comparable to the etching depth produced by a single laser shot ablation. To enhance the analytical capabilities of the method, we applied the collinear double-pulse LIBS technique, using a Michelson interferometer to split the laser pulse into two equal-energy pulses. Results obtained with Indium Tin Oxide (ITO) nanofilms (115 nm layer thickness) present a clear increase of the intensity emission by a factor of 3 to 10, depending on laser fluence, when the double-pulse approach is used. Single-pulse LIBS achieved an ablation rate of around 60 nm, while the double-pulse configuration achieved 40 nm/pulse, in a sequence of seven laser shots. Furthermore, via double-pulse LIBS spectra were recorded even at fluences as low as 150 mJ/cm 2, compared to 250 mJ/cm 2 required for capturing spectra, when the same total energy per pulse was maintained.