Andrew R. Mitchell | Searcharxiv

arXiv2024

Committor guided estimates of molecular transition rates

The probability that a configuration of a physical system reacts, or transitions from one metastable state to another, is quantified by the committor function. This function contains richly detailed mechanistic information about transition pathways, but a full parameterization of the committor requires building representing a high-dimensional function, a generically challenging task. Recent efforts to leverage neural networks as a means to solve high-dimensional partial differential equations, often called "physics-informed" machine learning, have brought the committor into computational reach. Here, we build on the semigroup approach to learning the committor and assess its utility for predicting dynamical quantities such as transition rates. We show that a careful reframing of the objective function and improved adaptive sampling strategies provide highly accurate representations of the committor. Furthermore, by directly applying the Hill relation, we show that these committors provide accurate transition rates for molecular system.

cond-mat.stat-mech↗

arXiv2021

Active Importance Sampling for Variational Objectives Dominated by Rare Events: Consequences for Optimization and Generalization

Deep neural networks, when optimized with sufficient data, provide accurate representations of high-dimensional functions; in contrast, function approximation techniques that have predominated in scientific computing do not scale well with dimensionality. As a result, many high-dimensional sampling and approximation problems once thought intractable are being revisited through the lens of machine learning. While the promise of unparalleled accuracy may suggest a renaissance for applications that require parameterizing representations of complex systems, in many applications gathering sufficient data to develop such a representation remains a significant challenge. Here we introduce an approach that combines rare events sampling techniques with neural network optimization to optimize objective functions that are dominated by rare events. We show that importance sampling reduces the asymptotic variance of the solution to a learning problem, suggesting benefits for generalization. We study our algorithm in the context of learning dynamical transition pathways between two states of a system, a problem with applications in statistical physics and implications in machine learning theory. Our numerical experiments demonstrate that we can successfully learn even with the compounding difficulties of high-dimension and rare data.

physics.data-an↗