Reactive Force Field Molecular Dynamics Study of the Effects of Gaseous Species on the Composition and Crystallinity of Silicon–Germanium Thin Films

Abstract

We simulated the growth of a silicon–germanium (SiGe) film using reactive force field molecular dynamics (ReaxFF MD) in combinations of SiH3, SiH2, GeH3, and GeH2 radicals to evaluate the effects of gaseous species on thin-film composition and crystallinity and to understand the growth mechanisms. The film compositions could be estimated in these combinations because of the linear increase in the Ge content of the films. The average crystallinity grown by SiH3 was higher than that by SiH2 radicals. The crystallinity of the film grown by SiH3 radicals tends to be drastically decreased by GeH2 radicals. The growth mechanisms for XH3 and XH2 (X = Si or Ge) radicals were compared. XH3 radicals abstracted surface H atoms, and then more XH3 radicals chemisorbed onto the formed dangling bonds, resulting in film growth through a two-step reaction known as the Eley–Rideal-type (ER-type) mechanism. The ER-type mechanism grows the film with a low hydrogen content and high crystallinity. In contrast, XH2 radicals displayed not only the ER-type mechanism but also a one-step reaction, the H-capturing mechanism, which incorporates surface H atoms into the gaseous species. The H-capturing mechanism results in film growth with high hydrogen content and low crystallinity. The growth mechanisms are influenced by high/low H-coverage. The surface H atoms thermally move around the bonded atoms and give their kinetic energy to the diffusing gaseous species. Excess surface H atoms promote desorption. Our results from the ReaxFF MD suggested experimental settings and conditions that would enable the growth of high-quality films. Our results also suggested that SiH3 and GeH3 radicals should be mainly generated in the gas phase for high-quality SiGe film growth.

Molecular analysis of hydrogen-bond structures in polymer electrolyte membrane in polymer electrolyte fuel cells below freezing temperatures

“…ReaxFF 12,13 MD simulations are able to consider the physical dynamics and chemical reactions simultaneously and is also used for such as analysis of semiconductor film formation processes. 14 In this research ReaxFF MD were performed with large-scale atomic/molecular massively parallel simulator (LAMMPS) 15 ReaxFF parameter was developed by Fantauzzi D. et al 16 In this simulation, we used 4 Nafion polymer chains, 40 hydronium ions, and 120 water molecules (water content: λ= 4). A periodic boundary condition was applied in the x, y, and z directions.…”