Efficient nonparametric $n$-body force fields from machine learning

TL;DR

This paper introduces a complete set of n-body Gaussian Process kernels for modeling interatomic forces, enabling efficient, accurate, and nonparametric force fields that outperform traditional methods in speed and flexibility.

Contribution

It provides explicit formulas for n-body GP kernels, a mapping to database-size-independent representations, and demonstrates their efficiency and accuracy in modeling atomic interactions.

Findings

n-body kernels can learn any interatomic interaction up to n-body contributions

3-body kernel reproduces forces with meV/Å accuracy

Mapped kernels are significantly faster and scalable

Abstract

We provide a definition and explicit expressions for $n$-body Gaussian Process (GP) kernels which can learn any interatomic interaction occurring in a physical system, up to $n$-body contributions, for any value of $n$. The series is complete, as it can be shown that the "universal approximator" squared exponential kernel can be written as a sum of $n$-body kernels. These recipes enable the choice of optimally efficient force models for each target system, as confirmed by extensive testing on various materials. We furthermore describe how the $n$-body kernels can be "mapped" on equivalent representations that provide database-size-independent predictions and are thus crucially more efficient. We explicitly carry out this mapping procedure for the first non-trivial (3-body) kernel of the series, and show that this reproduces the GP-predicted forces with $\text{meV/} \AA$ accuracy while being orders of magnitude faster. These results open the way to using novel force models (here named "M-FFs") that are computationally as fast as their corresponding standard parametrised $n$-body force fields, while retaining the nonparametric character, the ease of training and validation, and the accuracy of the best recently proposed machine learning potentials.