The H-1 and C-13 nuclear magnetic resonance (NMR) of thin diamond film
s deposited from naturally abundant (1.1 at. %) as well as 50% and 100
% C-13-enriched CH4 heavily diluted in H-2 is described and discussed.
Less than 0.6 at. % of hydrogen is found in the films which contain c
rystallites up to approximately 15 mum across. The H-1 NMR consists of
a broad 50-65-kHz-wide Gaussian line attributed to H atoms bonded to
carbon and covering the crystallite surfaces. A narrow Lorentzian line
was only occasionally observed and is found not to be intrinsic to th
e diamond structure. The C-13 NMR demonstrates that >99.5% of the C at
oms reside in a quaternary diamondlike configuration. H-1-C-13 cross-p
olarization measurement indicates that, at the very least, the majorit
y of C-13 nuclei cross polarized by H-1, i.e., within three bond dista
nces from a H-1 at a crystallite surface, reside in sp3 diamondlike co
ordinated sites. The C-13 relaxation rates of the films are four order
s of magnitude faster than that of natural diamond and believed to be
due to C-13 spin diffusion to paramagnetic centers, presumably carbon
dangling bonds. Analysis of the measured relaxation rates indicates th
at within the C-13 spin-diffusion length of square-root/DT1c approxima
tely 0.05 mum, these centers are uniformly distributed in the diamond
crystallites. The possibility that the dangling bonds are located at i
nternal nanovoid surfaces is discussed.