Abstract
Gallium arsenate (GaAsO4) has the highest piezoelectric properties among α-quartz-type materials. We describe first-principles calculations of the linear and second-order nonlinear optical properties of GaAsO4 combined with measurements of its second harmonic generation (SHG). Our calculations show that GaAsO4 has a SHG efficiency between 7.1 (LDA) and 12.3 pm/V (GGA), which is in agreement with our experiments (7.5 ± 1.5 pm/V) using the technique of Maker fringes. This SHG efficiency, attributed to an electronic transition from O 2p to As 4 s states, is higher than that observed in GaPO4 due to a better polarizability of As atoms. Thus, the thermal stability of GaAsO4 (no phase transition up to its thermal decomposition at 1303 K) associated with its high laser damage threshold (0.93 GW/cm2) make this compound a promising bifunctional material for piezoelectric and nonlinear optical applications at high temperatures.