Atomic-scale representation and statistical learning of tensorial properties

This chapter discusses the importance of incorporating three-dimensional symmetries in the context of statistical learning models geared towards the interpolation of the tensorial properties of atomic-scale structures. We focus on Gaussian process regression, and in particular on the construction of structural representations, and the associated kernel functions, that are endowed with the geometric covariance properties compatible with those of the learning targets. We summarize the general formulation of such a symmetry-adapted Gaussian process regression model, and how it can be implemented based on a scheme that generalizes the popular smooth overlap of atomic positions representation. We give examples of the performance of this framework when learning the polarizability and the ground-state electron density of a molecule

Recursive evaluation and iterative contraction of NN-body equivariant features

Mapping an atomistic configuration to an $N$-point correlation of a field associated with the atomic positions (e.g. an atomic density) has emerged as an elegant and effective solution to represent structures as the input of machine-learning algorithms. While it has become clear that low-order density correlations do not provide a complete representation of an atomic environment, the exponential increase in the number of possible $N$-body invariants makes it difficult to design a concise and effective representation. We discuss how to exploit recursion relations between equivariant features of different orders (generalizations of $N$-body invariants that provide a complete representation of the symmetries of improper rotations) to compute high-order terms efficiently. In combination with the automatic selection of the most expressive combination of features at each order, this approach provides a conceptual and practical framework to generate systematically-improvable, symmetry adapted representations for atomistic machine learning

Symmetry Regularization

The properties of a representation, such as smoothness, adaptability, generality, equivari- ance/invariance, depend on restrictions imposed during learning. In this paper, we propose using data symmetries, in the sense of equivalences under transformations, as a means for learning symmetry- adapted representations, i.e., representations that are equivariant to transformations in the original space. We provide a sufficient condition to enforce the representation, for example the weights of a neural network layer or the atoms of a dictionary, to have a group structure and specifically the group structure in an unlabeled training set. By reducing the analysis of generic group symmetries to per- mutation symmetries, we devise an analytic expression for a regularization scheme and a permutation invariant metric on the representation space. Our work provides a proof of concept on why and how to learn equivariant representations, without explicit knowledge of the underlying symmetries in the data.This material is based upon work supported by the Center for Brains, Minds and Machines (CBMM), funded by NSF STC award CCF-1231216

A Transferable Machine-Learning Model of the Electron Density

The electronic charge density plays a central role in determining the behavior of matter at the atomic scale, but its computational evaluation requires demanding electronic-structure calculations. We introduce an atom-centered, symmetry-adapted framework to machine-learn the valence charge density based on a small number of reference calculations. The model is highly transferable, meaning it can be trained on electronic-structure data of small molecules and used to predict the charge density of larger compounds with low, linear-scaling cost. Applications are shown for various hydrocarbon molecules of increasing complexity and flexibility, and demonstrate the accuracy of the model when predicting the density on octane and octatetraene after training exclusively on butane and butadiene. This transferable, data-driven model can be used to interpret experiments, initialize electronic structure calculations, and compute electrostatic interactions in molecules and condensed-phase systems

Invariance of visual operations at the level of receptive fields

Receptive field profiles registered by cell recordings have shown that mammalian vision has developed receptive fields tuned to different sizes and orientations in the image domain as well as to different image velocities in space-time. This article presents a theoretical model by which families of idealized receptive field profiles can be derived mathematically from a small set of basic assumptions that correspond to structural properties of the environment. The article also presents a theory for how basic invariance properties to variations in scale, viewing direction and relative motion can be obtained from the output of such receptive fields, using complementary selection mechanisms that operate over the output of families of receptive fields tuned to different parameters. Thereby, the theory shows how basic invariance properties of a visual system can be obtained already at the level of receptive fields, and we can explain the different shapes of receptive field profiles found in biological vision from a requirement that the visual system should be invariant to the natural types of image transformations that occur in its environment.Comment: 40 pages, 17 figure

Machine-learning of atomic-scale properties based on physical principles

We briefly summarize the kernel regression approach, as used recently in materials modelling, to fitting functions, particularly potential energy surfaces, and highlight how the linear algebra framework can be used to both predict and train from linear functionals of the potential energy, such as the total energy and atomic forces. We then give a detailed account of the Smooth Overlap of Atomic Positions (SOAP) representation and kernel, showing how it arises from an abstract representation of smooth atomic densities, and how it is related to several popular density-based representations of atomic structure. We also discuss recent generalisations that allow fine control of correlations between different atomic species, prediction and fitting of tensorial properties, and also how to construct structural kernels---applicable to comparing entire molecules or periodic systems---that go beyond an additive combination of local environments