Parameterizing complex reactive force fields using multiple objective evolutionary strategies (MOES). Part 1: ReaxFF...

ReaxFF (van Duin, A.C.T.; Dasgupta, S.; Lorant, F.; Goddard, W.A. J. Phys. Chem. A, 2001, 105, 9396-9409) reactive potentials are parametrized for cyclotrimethylene trinitramine (RDX) and 1,1-diamino-2,2-dinitroethene (FOX-7) in a novel application combining data envelopment analysis and a modern self-adaptive evolutionary algorithm to optimize multiple objectives simultaneously and map the entire family of solutions. In order to correct the poor crystallographic parameters predicted by ReaxFF using its base parametrization (Strachan, A.; van Duin, A. C. T.; Chakraborty, D.; Dasgupta S.; Goddard, W. A. Phys. Rev. Lett., 2003, 91, 098301), we augmented the existing training set data used for parametrization with additional (SAPT)DFT calculations of RDX and FOX-7 dimer interactions. By adjusting a small subset of the ReaxFF parameters that govern long-range interactions, the evolutionary algorithm approach converges on a family of solutions that best describe crystallographic parameters through simultaneous optimization of the objective functions. Molecular dynamics calculations of RDX and FOX-7 are conducted to assess the quality of the force fields, resulting in parametrizations that improve the overall prediction of the crystal structures.