Latent space design of interatomic potentials

Abstract

The advent of neural-network-based deep learning techniques has led to the emergence of increasingly sophisticated numerical interatomic potentials, including graph neural networks and large language-motivated foundation models. Parameterized to reproduce large, precomputed quantum mechanical training datasets for molecules and materials, models can be fine-tuned for greater accuracy on specific problems. Despite notable successes, machine learning (ML) models of potentials still face intrinsic challenges due to the combinatoric complexity of the underlying quantum chemical interactions, the existence of as-yet-undiscovered but potentially relevant bonding motifs absent from training datasets, and the need for post-prediction interpretability analysis. Drawing inspiration from autoencoder methods, we propose a constructive approach to interatomic potential design. In standard autoencoder architectures, a ML model self-organizes numerical training data in an unsupervised manner to discover underlying patterns and construct a compressed representation or latent space embedding model of the data, which is then used for prediction and inference. In the present work, we describe how latent space patterns and associated quantum embeddings can be constructed using first-principles methods based on theorems of density functional theory (DFT) and known, analytic constraints. This enables a parsimonious, physics-based representation of energies and densities, formally coupling the electronic and atomic length scales through the electron density, and linking ground, excited, and charge-transfer states of the interacting atoms. We describe the complete set of latent space components providing the foundation for a recently-proposed ensemble charge-transfer potential, and discuss opportunities for synergy in the design and explainability of contemporary machine-learned interatomic potentials.