화학공학소재연구정보센터
Journal of Physical Chemistry A, Vol.113, No.43, 11866-11881, 2009
Automatized Parametrization of SCC-DFTB Repulsive Potentials: Application to Hydrocarbons
In this work, we derive and test a new automatized strategy to construct repulsive potentials for the self-consistent charge density functional tight-binding (SCC-DFTB) method. This approach allows one to explore the parameter space in a systematic fashion in order to find optimal solutions. We find that due to the limited flexibility of the SCC-DFTB electronic part, not all properties can be optimized simultaneously. For example, the optimization of heats of formation is in conflict with the optimization of vibrational frequencies. Therefore, a special parametrization, for vibrational frequencies is derived. It is shown that the performance of SCC-DFTB can be significantly improved using a more elaborate fitting strategy. A new fit for C and H is presented, which results in an average error of 2.6 kcal/mol for heats of formations for a large set of hydrocarbons, indicating that the performance of SCC-DFTB can be systematically improved also for other elements.