Machine learning interatomic potentials (MLIPs) are a promising tool to accelerate atomistic simulations and molecular property prediction. The quality of MLIPs strongly depends on the quantity of available training data as well as the quantum chemistry (QC) level of theory used to generate that data. Datasets generated with high-fidelity QC methods, such as coupled cluster, are typically restricted to small molecules and may be missing energy gradients. With this limited quantity of data, it is often difficult to train good MLIP models. We present an ensemble knowledge distillation (EKD) method to improve MLIP accuracy when trained to energy-only datasets. In our EKD approach, first, multiple teacher models are trained to QC energies and then used to generate atomic forces for all configurations in the dataset. Next, a student MLIP is trained to both QC energies and to ensemble-averaged forces generated by the teacher models. We apply this workflow on the ANI-1ccx dataset which consists of organic molecules with configuration energies computed at the coupled cluster level of theory. The resulting student MLIPs achieve new state-of-the-art accuracy on the out-of-sample COMP6 benchmark and improved stability for molecular dynamics simulations. The EKD approach for MLIP is broadly applicable for chemical, biomolecular and materials science simulations.

Machine learning inter-atomic potentials (MLIPs) are revolutionizing the field of molecular dynamics (MD) simulations. Recent MLIPs have tended towards more complex architectures trained on larger datasets. The resulting increase in computational and memory costs may prohibit the application of these MLIPs to perform large-scale MD simulations. Here, we present a teacher-student training framework in which the latent knowledge from the teacher (atomic energies) is used to augment the students' training. We show that the light-weight student MLIPs have faster MD speeds at a fraction of the memory footprint compared to the teacher models. Remarkably, the student models can even surpass the accuracy of the teachers, even though both are trained on the same quantum chemistry dataset. Our work highlights a practical method for MLIPs to reduce the resources required for large-scale MD simulations.

Coarse-graining is a molecular modeling technique in which an atomistic system is represented in a simplified fashion that retains the most significant system features that contribute to a target output, while removing the degrees of freedom that are less relevant. This reduction in model complexity allows coarse-grained molecular simulations to reach increased spatial and temporal scales compared to corresponding all-atom models. A core challenge in coarse-graining is to construct a force field that represents the interactions in the new representation in a way that preserves the atomistic-level properties. Many approaches to building coarse-grained force fields have limited transferability between different thermodynamic conditions as a result of averaging over internal fluctuations at a specific thermodynamic state point. Here, we use a graph-convolutional neural network architecture, the Hierarchically Interacting Particle Neural Network with Tensor Sensitivity (HIP-NN-TS), to develop a highly automated training pipeline for coarse grained force fields which allows for studying the transferability of coarse-grained models based on the force-matching approach. We show that this approach not only yields highly accurate force fields, but also that these force fields are more transferable through a variety of thermodynamic conditions. These results illustrate the potential of machine learning techniques such as graph neural networks to improve the construction of transferable coarse-grained force fields.

We perform a set of flow and reactive transport simulations within three-dimensional fracture networks to learn the factors controlling mineral reactions. CO$_2$ mineralization requires CO$_2$-laden water, dissolution of a mineral that then leads to precipitation of a CO$_2$-bearing mineral. Our discrete fracture networks (DFN) are partially filled with quartz that gradually dissolves until it reaches a quasi-steady state. At the end of the simulation, we measure the quartz remaining in each fracture within the domain. We observe that a small backbone of fracture exists, where the quartz is fully dissolved which leads to increased flow and transport. However, depending on the DFN topology and the rate of dissolution, we observe a large variability of these changes, which indicates an interplay between the fracture network structure and the impact of geochemical dissolution. In this work, we developed a machine learning framework to extract the important features that support mineralization in the form of dissolution. In addition, we use structural and topological features of the fracture network to predict the remaining quartz volume in quasi-steady state conditions. As a first step to characterizing carbon mineralization, we study dissolution with this framework. We studied a variety of reaction and fracture parameters and their impact on the dissolution of quartz in fracture networks. We found that the dissolution reaction rate constant of quartz and the distance to the flowing backbone in the fracture network are the two most important features that control the amount of quartz left in the system. For the first time, we use a combination of a finite-volume reservoir model and graph-based approach to study reactive transport in a complex fracture network to determine the key features that control dissolution.