Growth, doping, andin situetching of GaAs using cracked and uncracked tris-dimethylaminoarsenic (TDMAAs) in chemical beam epitaxy (CBE) have been studied. A reflection high-energy electron diffraction study indicates that the complete decomposition of TDMAAs occurs below370 °C. Possible TDMAAs decomposition pathways, which are consistent with experimental data, are presented. The carbon level in undoped GaAs films and the hole concentration in carbon-doped GaAs films using uncracked TDMAAs are much lower than those using cracked TDMAAs, which may be due to atomic hydrogen released from theβ-hydride elimination process of uncracked TDMAAs on the GaAs surface. Thein situGaAs etching effect was observed only when the substrate was exposed to uncracked TDMAAs. Possibly, reactive free radicals generated by uncracked TDMAAs on GaAs surfaces are responsible for the etching effect. Surface roughness in selective-area growth of GaAs and the poor interfaces in InGaAs/GaAs multiple quantum wells grown by CBE using uncracked TDMAAs may result from this etching effect.