Interaction of high intensity optical pulses with modified nonlinear GaSe crystals

The modified Bridgman method with heat field rotation was used to grow epsilon-polytype single crystals of pure and 1, 2 and 10 mass % S-doped GaSe or solid solution crystals GaSe1-xSx, x = 0.002, 0.091, 0.412. The interaction of ultrashort laser pulses of similar to 100 fs duration at 800 nm and 2 mu m with the grown crystals was studied at room temperature. Up to 3.4-fold advantage of S-doped crystals in limit pump intensity (no decrease in the transmission) was found under 800 nm pump at S-content increase up to 10 mass %. The advantage became a half less at 2 mu m pump due to a decrease of two-photon absorption in pure GaSe crystals. The spectral dependence of transient absorption is recorded with 37 fs resolution and interpreted. It was ascertained that first observable damage of high quality crystals is caused by dissociation of sub-micrometer thick surface layer to initial elements and do not influence the frequency conversion efficiency until alloying of dissociated Ga. Local microdefects, multiphoton absorption and transient transmission processes are identified as key factors responsible for damage threshold.