The immense promise of linear scaling electronic structure theory to enable computational studies of complex materials directly from the fundamental principles of quantum mechanics has never been fully realized because of a number of shortcomings, in particular, (a) the accuracy is reduced to a level that is often difficult, if not impossible, to control; (b) the computational pre-factor is high and the linear scaling benefit occurs only for very large systems that in practice often are beyond acceptable time limits or available computer resources; and (c) the parallel performance is generally challenged by a significant overhead and the wall-clock time remains high even with massive parallelism. These obstacles are particularly limiting in quantum-based Born-Oppenheimer molecular dynamics simulations, where we currently are constrained either to small system sizes or to very short simulation times. We show how graph theory can be combined with quantum theory to overcome major bottlenecks and be used to calculate the electronic structure of large complex systems with well-controlled accuracy and natural low-communication parallelism. This brings quantum mechanical, nanosecond-duration Born-Oppenheimer molecular dynamics simulations of biomolecules and other extensive systems within practical reach.

Graph-based linear scaling electronic structure theory for Born-Oppenheimer molecular dynamics

254th National Meeting (2017)

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