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The porous silicon (PS) surface modification diagnostics due to functionalization and water adsorption/desorption processes were provided by the self-action effects of picosecond range pulsed laser radiation at 1064 nm. It was shown that the PS surface functionalization—oxide removal, alkylation, and oxidation—resulted in a refractive nonlinear optical (NLO) response sign turn to self-focusing (Δn...