The role of defects on the transition from saturable absorption to nonlinear absorption of Bi₁₂GeO₂₀ single crystal under increasing laser excitation

Abstract

This work reports defect and input intensity dependent nonlinear optical behaviors of Bi12GeO20 (BGO) single crystal. Open aperture (OA) Z-scan experiments were performed with 532 nm excitation wavelength under 4 ns and 100 fs pulsed laser irradiation. Obtained data were fitted with a theoretical model considering one-photon, two-photon and free carrier absorption contributions to nonlinear absorption due to longer lifetime of localized defect states than that of used laser pulse durations. At low input intensities, the BGO single crystal showed saturable absorption (SA) behavior and transition to nonlinear absorption (NA) behavior observed with further increase of the input intensities both of pulse durations. At low input intensity, the OPA mechanism is dominant and results in SA by filling of the defect states due to defect state at around one photon energy (2.32 eV). At higher input intensity, multi-photon, two-photon and free carrier absorption become dominant mechanisms, and nonlinear absorption behavior was observed. The lowest saturation threshold was found as 1.36 x 1010 W/cm2 with nanosecond pulses. We have revealed the mechanisms contributing both SA and NA, and determined saturation intensity threshold and effective nonlinear absorption coefficients. Our findings indicate that the tails of defect states overlap in the energy band gaps especially in sufficiently disordered crystal. With this way, the spectral range for saturable absorption and nonlinear absorption can be broadened.