Journal of Crystal Growth, Vol.397, 29-38, 2014
Hydrothermal growth of large piezoelectric single crystals of GaAsO4
GaAsO4 crystals were grown by a hydrothermal epitaxial process. Micro crystalline GaAsO4 powder was first synthesized by hydrothermal methods by using GaAs as a starting material in a sulfuric acid solvent under oxidizing conditions. Experimental conditions were optimized and the yield of the nutrient synthesis reached 88%. GaAsO4 powder was then used as the nutrient for growing GaAsO4 single crystals by epitaxy on (2(1) over bar 0) oriented GaPO4, AlPO4 and GaAsO4 plates. Crystal growth was performed in a horizontal PTFE-lined autoclave divided into two parts using sulfuric acid as the solvent under a slow heating gradient. Hydrothermal conditions were optimized in order to improve the crystal quality. The influence of the nature and orientation of the seeds on the growth rate was studied. From the solubility curve, the solute supply Delta S as a function of temperature during the growth process was calculated. Transparent crystals were obtained with Delta S between 0.002 and 0.009 mol/L. Large crystals (3.9 Chi 1.8 Chi 1.4 cm(3)) of gallium arsenate were obtained. These crystals were cut into (2(1) over bar 0), (010) and (001) plates. Mapping using Raman spectroscopy was performed in order to study the growth recovery on the seed. GaAsO4 crystals were characterized by infrared spectroscopy in order to quantify the amount of OH groups in the crystal structure. A low value of the absorption coefficient a at 3300 cm(-1) was measured 0.067 cm(-1) indicating a good crystal quality. Optical measurements were performed on GaAsO4 crystals by UV-vis-NIR spectrophotometry. Gallium arsenate exhibits the highest value of birefringence in the alpha-quartz group with Delta n =0.033. The transmission in the spectral region above 250 nm yields a bandgap of 5.85 eV. Piezoelectric properties were measured on resonators. An electromechanical coupling coefficient of 20% was measured which is the highest in the alpha-quartz group. A quality factor QF of 3.2 Chi 10(10) was obtained on a Y-cut plate. The C-66 elastic constant was found to be 20 GPa. (C) 2014 Elsevier B.V. All rights reserved.
Keywords:Solubility;Hydrothermal crystal growth;Single crystal growth;Growth from solutions;Arsenates;Piezoelectric materials