We
redeveloped the ReaxFF force field parameters for Si/O/H interactions
that enable molecular dynamics (MD) simulations of Si/SiO2 interfaces and O diffusion in bulk Si at high temperatures, in particular
with respect to point defect stability and migration. Our calculations
show that the new force field framework (ReaxFFpresent),
which was guided by the extensive quantum mechanical-based training
set, describes correctly the underlying mechanism of the O-migration
in Si network, namely, the diffusion of O in bulk Si occurs by jumping
between the neighboring bond-centered sites along a path in the (110)
plane, and during the jumping, O goes through the asymmetric transition
state at a saddle point. Additionally, the ReaxFFpresent predicts the diffusion barrier of O-interstitial in the bulk Si
of 64.8 kcal/mol, showing a good agreement with the experimental and
density functional theory values in the literature. The new force
field description was further applied to MD simulations addressing
O diffusion in bulk Si at different target temperatures ranging between
800 and 2400 K. According to our results, O diffusion initiates at
the temperatures over 1400 K, and the atom diffuses only between the
bond-centered sites even at high temperatures. In addition, the diffusion
coefficient of O in Si matrix as a function of temperature is in overall
good agreement with experimental results. As a further step of the
force field validation, we also prepared amorphous SiO2 (a-SiO2) with a mass density of 2.21 gr/cm3, which excellently agrees with the experimental value of 2.20 gr/cm3, to model a-SiO2/Si system. After annealing the
a-SiO2/Si system at high temperatures until below the computed
melting point of bulk Si, the results show that ReaxFFpresent successfully reproduces the experimentally and theoretically defined
diffusion mechanism in the system and succeeded in overcoming the
diffusion problem observed with ReaxFFSiOH(2010), which
results in O diffusion in the Si substrate even at the low temperature
such as 300 K.