Films are deposited on a substrate by a process in which
atomic layer deposition (ALD) is used to deposit one layer of the film and pulsed
chemical vapor deposition (CVD) is used to deposit another layer of the film. During the ALD part of the process, a layer is formed by flowing sequential and alternating pulses of mutually reactive reactants that deposit self-limitingly on a substrate. During the pulsed CVD part of the process, another layer is deposited by flowing two CVD reactants into a
reaction chamber, with at least a first of the CVD reactants flowed into the
reaction chamber in pulses, with those pulses overlapping at least partially with the flow of a second of the CVD reactants. The ALD and CVD parts of the process ca be used to deposit
layers with different compositions, thereby forming, e.g., nanolaminate films. Preferably, high quality
layers are formed by flowing the second CVD reactant into the
reaction chamber for a longer total duration than the first CVD reactant. In some embodiments, the pulses of the third reactant at separated by a duration at least about 1.75 times the length of the pulse. Preferably, less than about 8 monolayers of material are deposited per pulse of the first CVD reactant.