Theoretical predictions using a modified radical species ternary diagram for C-H-O system indicate that addition of sulfur expands the C-H-O gas phase compositional window for diamond deposition. Sulfur addition to no-growth domain increases the carbon super-saturation by binding the oxygen and the addition of sulfur to the non-diamond domain reduces the heavy carbon super-saturation by decreasing CnHm species concentration in the gas phase. The overall effect of sulfur addition to gas phase mixtures is characterized as that of oxygen addition to the C-H system, i.e. expansion of the compositional window over which diamond can be deposited from the gas phase. In addition, the increasing sulfur concentration to diamond domain feed gases beyond 2000 ppm did not affect the steady state gas phase composition but the quality of diamond was reduced. (C) 2003 Elsevier B.V. All rights reserved.