| Summary: | Two-photon absorption has been systematically studied in Ca<sub>3</sub>(VO<sub>4</sub>)<sub>2</sub> and Ca<sub>2.7</sub>Sr<sub>0.3</sub>(VO<sub>4</sub>)<sub>2</sub> crystals, both of which are prospective nonlinear optical and laser host materials. A strong dependence of the two-photon absorption coefficients on the orientation of the laser beam polarization with respect to the optical c-axis of the crystals is revealed. The measured coefficients for perpendicular and parallel orientations were 50 ± 10 cm/TW and 19 ± 4 cm/TW in Ca<sub>3</sub>(VO<sub>4</sub>)<sub>2</sub>, and 18 ± 3 cm/TW and 10 ± 2 cm/TW in Ca<sub>2.7</sub>Sr<sub>0.3</sub>(VO<sub>4</sub>)<sub>2</sub>, respectively. Thus, to minimize optical losses caused by two-photon absorption, an orientation of Ca<sub>2.7</sub>Sr<sub>0.3</sub>(VO<sub>4</sub>)<sub>2</sub> crystals with the laser beam polarization parallel to the crystal optical c-axis is preferred.
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