Abstract: Sequential processes are conducted in a batch reaction chamber to form ultra high quality silicon-containing compound layers, e.g., silicon nitride layers, at low temperatures. Under reaction rate limited conditions, a silicon layer is deposited on a substrate using trisilane as the silicon precursor. Trisilane flow is interrupted. A silicon nitride layer is then formed by nitriding the silicon layer with nitrogen radicals, such as by pulsing the plasma power (remote or in situ) on after a trisilane step. The nitrogen radical supply is stopped. Optionally non-activated ammonia is also supplied, continuously or intermittently. If desired, the process is repeated for greater thickness, purging the reactor after each trisilane and silicon compounding step to avoid gas phase reactions, with each cycle producing about 5-7 angstroms of silicon nitride.