Revealing photoluminescence and nonlinear optical absorption characteristics of PbMo_0.75W_0.25O₄ single crystal for optical limiting applications

Abstract

Nonlinear absorption properties of PbMo0.75W0.25O4 single crystal fabricated by the Czochralski method were studied. The band gap energy of the crystal was determined as 3.12 eV. Urbach energy which represents the defect states inside the band gap was found to be 0.106 eV. PbMo0.75W0.25O4 single crystal has a broad photoluminescence emission band between 376 and 700 nm, with the highest emission intensity occurring at 486 nm and the lowest intensity peak at 547 nm, depending on the defect states. Femtosecond transient absorption measurements reveal that the lifetime of localized defect states is found to be higher than the 4 ns pulse duration. Open aperture (OA) Z-scan results demonstrate that the PbMo0.75W0.25O4 single crystal exhibits nonlinear absorption (NA) that includes two-photon absorption (TPA) as the dominant mechanism at the 532 nm excitations corresponding to 2.32 eV energy. NA coefficient (beta(eff)) increased from 7.24 x 10(-10) m W-1 to 8.81 x 10(-10) m W-1 with increasing pump intensity. At higher intensities beta(eff) tends to decrease with intensity increase. This decrease is an indication that saturable absorption (SA) occurred along with the TPA, called saturation of TPA. The lifetime of the defect states was measured by femtosecond transient absorption spectroscopy. Saturable absorption behavior was observed due to the long lifetime of the localized defect states. Closed aperture (CA) Z-scan trace shows the sign of a nonlinear refractive index. The optical limiting threshold of PbMo0.75W0.25O4 single crystal at the lowest intensity was determined as 3.45 mJ/cm(2). Results show that the PbMo0.75W0.25O4 single crystal can be a suitable semiconductor material for optical limiting applications in the visible region.