Long-Time Dynamics through Parallel Trajectory Splicing

• Published in: Journal of chemical theory and computation 2016-01, Vol.12 (1), p.18-28
• Main Authors: Perez, Danny, Cubuk, Ekin D, Waterland, Amos, Kaxiras, Efthimios, Voter, Arthur F
• Format: Article
• Language: English
• Subjects: Computation; Computational efficiency; Computer simulation; Dynamics; Evolution; Splicing; Strategy; Trajectories
• ISSN: 1549-9618; 1549-9626
• DOI: 10.1021/acs.jctc.5b00916

Simulating the atomistic evolution of materials over long time scales is a longstanding challenge, especially for complex systems where the distribution of barrier heights is very heterogeneous. Such systems are difficult to investigate using conventional long-time scale techniques, and the fact that they tend to remain trapped in small regions of configuration space for extended periods of time strongly limits the physical insights gained from short simulations. We introduce a novel simulation technique, Parallel Trajectory Splicing (ParSplice), that aims at addressing this problem through the timewise parallelization of long trajectories. The computational efficiency of ParSplice stems from a speculation strategy whereby predictions of the future evolution of the system are leveraged to increase the amount of work that can be concurrently performed at any one time, hence improving the scalability of the method. ParSplice is also able to accurately account for, and potentially reuse, a substantial fraction of the computational work invested in the simulation. We validate the method on a simple Ag surface system and demonstrate substantial increases in efficiency compared to previous methods. We then demonstrate the power of ParSplice through the study of topology changes in Ag42Cu13 core–shell nanoparticles.