We have grown thin layers of gamma'Fe4N on Cu(100) substrates by molecular beam epitaxy in a flow of atomic nitrogen, delivered by a radio-frequency (RF) plasma source. This nitride phase is a ferromagnetic metallic conductor and has interesting properties for device applications. In addition it has an intriguing growth mechanism. In earlier work we found that pure crystalline layers can be grown at substrate temperatures higher than 250degreesC, with excess nitrogen and in the presence of hydrogen.(1) To gain insight into the growth mechanism, we studied the structure and composition with scanning tunneling microscopy (STM), Auger electron spectroscopy (AES), low-energy electron diffraction (LEED) and X-ray diffraction (XRD). This was done...