We are studying carbon thin films by using a pulsed excimer laser to ablate pyrolytic graphite targets to form highly tetrahedral coordinated amorphous carbon (at-C) films. These films have been grown on room temperature p-type Si (100) substrates without the intentional incorporation of hydrogen. In order to understand and optimize the growth of at-C films, parametric studies of the growth parameters have been performed. We have also introduced various background gases (H2, N2 and Ar) and varied the background gas pressure during deposition. The residual compressive stress levels in the films have been measured and correlated to changes in the Raman spectra of the at-C band near 1565 cm−1. The residual compressive stress falls with gas pressure, indicating a decreasing atomic sp3-bonded carbon fraction. We find that reactive gases such as hydrogen and nitrogen significantly alter the Raman spectra at higher pressures. These effects are due to a combination of chemical incorporation of nitrogen and hydrogen into the film as well as collisional cooling of the ablation plume. In contrast, films grown in non-reactive Ar background gases show much less dramatic changes in the Raman spectra at similar pressures.