| 研究実績の概要 |
The goal of this project was to develop a method capable of performing accelerated quantum chemical simulations to simulate chirality-controlled single-walled carbon nanotube (SWCNT) growth. As a first step towards this goal, we had reported the development of the GRRM-DFTB-based fly-KMC method. We have reported this method in a peer-reviewed paper in the 2016 fiscal year: I. Mitchell, S. Irle,* A. J. Page,* A Global Reaction Route Mapping-based Kinetic Monte Carlo Algorithm, J. Chem. Phys. 145(2), 024105/1-8 (2016). We are presently improving the performance of this methodology, as even the simulation of a single carbon atom diffusion on an iron nanoparticle turned out to become computationally highly expensive. Nevertheless, we succeeded to show that the GRRM-KMC method is capable of reproducing the 1st order kinetics observed during independent quantum chemical molecular dynamics simulations using the DFTB potential.
Although GRRM can be used as a basis for exhaustively searching for all stationary points on a molecular PES, our approach truncates the GRRM search to a single local minimum. The TSs identified by the truncated GRRM search are then used to construct an on-the-fly move table, which is applied during a subsequent KMC time propagation step. We demonstrate the efficacy of this algorithm on model systems pertinent to two archetypal chemical reactions - intramolecular proton transfer and nanoscale surface diffusion.
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