Fast method for quantum mechanical molecular dynamics

Abstract

With the continuous growth of processing power for scientific computing, first principles Born-Oppenheimer molecular dynamics (MD) simulations are becoming increasingly popular for the study of a wide range of problems in materials science, chemistry and biology. Nevertheless, the computational cost still remains prohibitively large in many cases, particularly in comparison to classical MD simulations using empirical force fields. Here we show how to circumvent the major computational bottleneck in Born-Oppenheimer MD simulations arising from the self-consistent-charge optimization. The optimization-free quantum mechanical MD method is demonstrated for density functional tight-binding theory. The molecular trajectories are almost indistinguishable from an "exact" microcanonical Born-Oppenheimer MD simulation even when linear scaling sparse matrix algebra is used. Our findings drastically reduce the computational gap between classical and quantum mechanical MD simulations.

12 pages, 7 figures

References in corpus (3)

• An Efficient and Accurate Car-Parrinello-like Approach to Born-Oppenheimer Molecular Dynamics
• Time-reversible Born-Oppenheimer molecular dynamics
• Efficient formalism for large scale ab initio molecular dynamics based on time-dependent density functional theory

Cited by in corpus (10)

• Generalized Extended Lagrangian Born-Oppenheimer Molecular Dynamics
• First principles molecular dynamics without self-consistent field optimization
• Analysis of the Time Reversible Born-Oppenheimer Molecular Dynamics
• Accelerating Wave Function Convergence in Interactive Quantum Chemical Reactivity Studies
• On the existence of the optimal order for wavefunction extrapolation in Born-Oppenheimer molecular dynamics
• Adiabatic motion and statistical mechanics via mass zero constrained dynamics
• Extended Lagrangian Born-Oppenheimer molecular dynamics in the limit of vanishing self-consistent field optimization
• Bringing discrete-time Langevin splitting methods into agreement with thermodynamics
• Convergence of Stochastic-extended Lagrangian molecular dynamics method for polarizable force field simulation
• Accelerated density matrix expansions for Born-Oppenheimer molecular dynamics