Atomic layer epitaxy (ALE) of GaAs using triethylgallium (TEG) with the combination of arsine has been limited to an extremely narrow temperature range. It is demonstrated that the temperature range for ALE using TEG is substantially expanded when arsine is replaced with an alkyl‐As, tris‐dimethylamino‐arsenic {As[N(CH3)2]3}. The role of the As source materials on the self‐limiting mechanism is discussed with the measurement of the surface reaction species employing a transient quadrupole mass spectrometry.

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