Radiofrequency (RF) nitrogen plasma sources are commonly used for the growth of III-nitrides by plasma-assisted molecular beam epitaxy. Their output mainly consists of a mixture of atomic nitrogen and metastable excited molecules. The relative concentration of these species as a function of RF power and nitrogen gas flow rate has been investigated by plasma optical emission spectroscopy. It is shown that the concentration of excited molecular nitrogen species is monotonically increasing with both parameters while the concentration of nitrogen atoms is almost independent of the nitrogen gas flow rate and increases monotonically with the coupled RF power. As a result of this functional dependence, the plasma source can be tuned to produce mainly excited nitrogen molecules or a mixture of excited molecules and atomic nitrogen. Comparison of the growth rates of gallium nitride films grown under different operating conditions of the RF source with the optical spectroscopy data shows that the metastable excited nitrogen molecules component of the source is the predominant factor contributing in the III-nitrides growth. © 2005 Elsevier B.V. All rights reserved.