We report on the preparation of hydrogen-free nanocrystalline diamond films by pulsed electron beam ablation (channel-spark) from a single target on silicon and stainless steel substrates and under different process conditions. The films have been grown from highly ordered pyrolytic graphite at room temperature in an argon atmosphere under a pressure of 0.6 Pa. This study aims at elucidating the influence of the accelerating voltage (13, 14.5, and 16 kV) and electron beam pulse repetition rate (5 and 8 Hz) on film morphology, grain size, carbon-carbon sp 3 content, and crystalline fraction. The films have been characterized using visible-reflectance spectroscopy, visible-Raman spectroscopy, scanning electron microscopy (SEM), and atomic force microscopy (AFM). The correlations between measurement data and film properties are examined and discussed.Diamond has a set of technologically attractive properties such as its extraordinarily high hardness and thermal conductivity, low friction coefficient, high stiffness, excellent electrical resistivity, high energy-bandgap, and excellent chemical stability. The preparation of artificial diamond has been an ongoing effort for over 100 years. One early and tangible effort is due to Hershey, in late 1920s, who claimed to have made diamond from the rapid freezing of excess carbon dissolved in molten iron. 1 Many attempts have ensued, which are based on high-pressure and high-temperature conditions and culminated in the commercial synthesis of diamond from graphite by ASEA in Sweden 2 and General Electric. 3 In the early 1960s, diamond films were produced by the pyrolysis of methane over a diamond substrate. 4 Further successful attempts, throughout the 1970s-1980s, have been reported at producing films of diamond via chemical vapor deposition (CVD) from carbonaceous gas mixtures and hydrogen (or other halogens), e.g., see 5,6 for a comprehensive account. The growth of diamond films continues to attract intensive worldwide attention by the research community, as high-quality films exhibit most of the unsurpassed properties of natural diamond and they are much more cost effective.Nanocrystalline diamond (NCD) is a nano-composite consisting of nanometer-sized diamond crystallites, which are surrounded by an amorphous carbon matrix. The diamond crystallites are made up of sp 3 hybridized carbon bonded atoms, while the amorphous carbon phase consists of both sp 3 and sp 2 hybridized carbon atoms (and eventually hydrogen, in case of deposition in a hydrogen-rich atmosphere). The interfacial region of these two phases consists of a less-distinguishable phase or the grain boundaries. The latter and the amorphous carbon matrix could be considered as one phase due to the small volumes, i.e., < 10%, of the amorphous carbon regions. 7,8 NCD films, with their smooth surface and high sp 3 C-C bond content, are promising candidates in a broad range of applications, such as such as in optics, tribology, biomedicine, and catalysis. 9,10 In addition to CVD methods, the growth of films of dia...