Modelling of ZrO2 deposition from ZrCl4 and H2O on the Si(1 0 0) surface: initial reactions and surface structures

The mechanism of initial reactions and atomic structures arising in ZrO2 atomic layer deposition (ALD) on a Si(1 0 0) substrate using ZrCl4 and H2O as precursors have been studied using first-principle DFT plane-wave and quantum-chemical cluster calculations. The wet oxidation of silicon and reactions corresponding to the first two ZrO2 ALD steps have been examined, and energy characteristics of these reactions have been calculated in the cluster approximation. The results of cluster and periodic calculations have been compared. The growth of amorphous ZrO2 films has been explained based on a simple chemical mechanism.