A DFT study on the reaction mechanism of aluminum film growth by CVD
Masashi. Nakatomi(

),T. Nakajima and K. Yamashita
Dept. of Chemical System Engineering, The University of Tokyo.
We carried out ab initio density functional calculations about elementary
reactions, which are constituents of Al-CVD. Calculated rate constants and
their temperature dependency were employed to clarify the reaction mechanism.
In this work, we studied Al-film growth on an Al(111) surface using DMEAA
(dimethyl-ethyl amine alane) as source gas. In the previous work, we have
found that DMEAA once get adsorbed to the surface and then only DMEA
dissociates from the surface. We therefore concentrated on several elementary
reactions on the surface supposed to occur from alane molecules. We attached
an alane molecule to a cluster constituted of eighteen Al atoms. The energy
diagrams for each elementary reaction were calculated based on the fully
optimized structures of reactants, transition states, and products. All
calculations were carried out with the density functional theory (DFT) at the
level of B3P86/LanL2DZ. Then we obtained the rate constants by the transition
state theory with quantum tunneling correction.
We have found that the adsorbed alane molecules dissociate to AlH and two
hydrogen atoms on the surface, and that H atoms are easily desorbed from the
surface as gas-phased hydrogen molecules. We may conclude that Al-films grow
by the desorption of H after the cohesion of AlH. The rate constants obtained
in this study will be utilized to calculate the film growth rate in kinetic
study.