Pushing the limits of Multiple-Timestep Strategies for Polarizable Point Dipole Molecular Dynamics

We propose an incremental construction of multi-time-step integrators to accelerate polarizable point dipole molecular dynamics while preserving sampling efficiency. We start by building integrators using frequency-driven splittings of energy terms and a Velocity-Verlet evaluation of the most rapidly varying forces and compare a standard bonded/nonbonded split to a three-group split dividing nonbonded forces (including polarization) into short- and long-range contributions. We then introduce new approaches by coupling these splittings to Langevin dynamics and to Leimkuhler’s BAOAB integrator in order to reach larger time steps (6 fs) for long-range forces. We further increase sampling efficiency by (i) accelerating the polarization evaluation using a fast/noniterative truncated conjugate gradient (TCG-1) as a short-range solver and (ii) pushing the outer time step to 10 fs using hydrogen mass repartitioning. The new BAOAB-RESPA1 integrators demonstrate up to a 7-fold acceleration over standard 1 fs (Tinke...