Low-pressure diamond deposition from hydrocarbon/hydrogen ps-phase mix
tures was discovered over 20 years ago, but the exact deposition mecha
nism remained unknown. Work reported here confirms preferential graphi
te erosion to be the rate-controlling step, as had been assumed by som
e researchers earlier, and identifies reaction pathways by which the g
raphitic constituents of the deposit are preferentially removed. Model
systems of C:H a few monolayers thick were used to show that dehydrog
enation, erosion, and hydrogenation all play a part.