Stochastic Constrained Extended System Dynamics for Solving Charge Equilibration Models

SC Tan and I Leven and D An and L Lin and T Head-Gordon, JOURNAL OF CHEMICAL THEORY AND COMPUTATION, 16, 5991-5998 (2020).

DOI: 10.1021/acs.jctc.0c00514

We present a new stochastic extended Lagrangian molecular dynamics solution to charge equilibration that eliminates self-consistent field (SCF) calculations, thus eliminating the computational bottleneck in solving the charge distribution with standard SCF solvers. By formulating both charges and chemical potential as latent variables and introducing a holonomic constraint that satisfies charge conservation, the SC-XLMD method accurately reproduces thermodynamic, dynamic, and structural properties within the framework of ReaxFF for a bulk water system and highly reactive RDX molecules simulated at high temperature. The SC-XLMD method shows excellent computational performance and is available in the publicly available LAMMPS package.

Return to Publications page