Larentzos James P, Rice Betsy M, Byrd Edward F C, Weingarten N Scott, Lill James V
Engility Corporation, High Technology Services Group, U.S. Army Research Laboratory , Aberdeen Proving Ground, Maryland 21005, United States.
Energetic Materials Science Branch, Weapons and Materials Research Directorate, U.S. Army Research Laboratory , Aberdeen Proving Ground, Maryland 21005, United States.
J Chem Theory Comput. 2015 Feb 10;11(2):381-91. doi: 10.1021/ct500788c.
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.
ReaxFF（范·杜因，A.C.T.；达斯古普塔，S.；洛兰特，F.；戈达德，W.A.《物理化学杂志A》，2001年，第105卷，9396 - 9409页）反应势针对环三亚甲基三硝胺（RDX）和1,1 - 二氨基 - 2,2 - 二硝基乙烯（FOX - 7）进行了参数化，这是一种将数据包络分析与现代自适应进化算法相结合的新颖应用，可同时优化多个目标并绘制整个解集族。为了校正ReaxFF使用其基本参数化预测的较差晶体学参数（斯特拉坎，A.；范·杜因，A.C.T.；恰克拉波蒂，D.；达斯古普塔，S.；戈达德，W.A.《物理评论快报》，2003年，第91卷，098301），我们用RDX和FOX - 7二聚体相互作用的额外（SAPT）DFT计算扩充了用于参数化的现有训练集数据。通过调整控制长程相互作用的一小部分ReaxFF参数，进化算法方法收敛于一族通过同时优化目标函数能最佳描述晶体学参数的解。对RDX和FOX - 7进行了分子动力学计算以评估力场的质量，从而得到能改善晶体结构整体预测的参数化。
