Single‐crystal , , and films have been grown on and a number of insulating substrates by the decomposition of alkyl‐gallium compounds in the presence of arsine, phosphine, arsine‐phosphine, and arsine‐stibine mixtures. Both triethylgallium and trimethylgallium have been used successfully in the preparation of . This process makes compound semiconductor film growth compatible with methods used for the growth of elemental semiconductors and eliminates many of the difficulties inherent in multitemperature‐zone processes.