The heterogrowth of diamond on Si(100) using individual atomic H and m
ethyl molecular beams under high vacuum conditions has been investigat
ed using in situ X-ray photoelectron and associated electron energy lo
ss spectroscopies, along with Raman spectroscopy and secondary electro
n microscopy. Reaction of the methyl molecular beam along with the hea
ted Si surface is shown to provide an efficient route for the formatio
n of SiC and graphitic carbon phases, which are etched away only slowl
y using the atomic H beam. Atomic hydrogen inhibits the formation of t
hese phases when both beams simultaneously interact with the heated su
rface. Diamond films can nonetheless be deposited provided the methyl:
hydrogen flux ratios are not too low and some of the characteristics o
f this molecular beam approach to thin film diamond are discussed.