We have investigated a possibility of the site-controlled InGaAsN epitaxy by using a new source material of hexakis-diethviamido-diiiidium ([In{N(C2H5)(2)}(3)](2)). In the site-controlled epitaxy of the InGaAsN layer, the N atoms should be incorporated randomly and should also preferentially form In-N bonds during growth. The new source has been developed to satisfy these two requirements for the site-controlled epitaxy. Single-crystalline InN layer has been successfully obtained on a nitrided α-Al2O3 Substrate by supplying only a [In{N(C2H5)(2)}(3)](2) beam. Polycrystalline InNAs has also been obtained on a nitrided α-Al2O3 substrate by [In{N(C2H5)(2)}(3)](2) and an As-4 beam supplied simultaneously. Furthermore, phase separation into GaAs and InN phases has been observed in the layers grown under simultaneous irradiation of Ga, As-4 and [In{N(C2H5)(2)}(3)](2) beams on a nitrided α-Al2O3 substrate. The results strongly indicate that site-controlled epitaxy can be expected to be achieved by using new source materials, such as [In{N(C2H5)(2)}(3)](2) that can produce the In N fragments efficiently. © 2004 Elsevier B.V. All rights reserved.