Autotuning T-PaiNN: Enabling Data-Efficient GNN Interatomic Potential Development via Classical-to-Quantum Transfer Learning

Machine-learned interatomic potentials (MLIPs), particularly graph neural network (GNN)-based models, offer a promising route to achieving near-density functional theory (DFT) accuracy at significantly reduced computational cost. However, their practical deployment is often limited by the large volumes of expensive quantum mechanical training data required. In this work, we introduce a transfer learning framework, Transfer-PaiNN (T-PaiNN), that substantially improves the data efficiency of GNN-MLIPs by leveraging inexpensive classical force field data. The approach consists of pretraining a PaiNN MLIP architecture on large-scale datasets generated from classical molecular simulations, followed by fine-tuning (dubbed autotuning) using a comparatively small DFT dataset. We demonstrate the effectiveness of autotuning T-PaiNN on both gas-phase molecular systems (QM9 dataset) and condensed-phase liquid water. Across all cases, T-PaiNN significantly outperforms models trained solely on DFT data, achieving order-of-magnitude reductions in mean absolute error while accelerating training convergence. For example, using the QM9 data set, error reductions of up to 25 times are observed in low-data regimes, while liquid water simulations show improved predictions of energies, forces, and experimentally relevant properties such as density and diffusion. These gains arise from the model's ability to learn general features of the potential energy surface from extensive classical sampling, which are subsequently refined to quantum accuracy. Overall, this work establishes transfer learning from classical force fields as a practical and computationally efficient strategy for developing high-accuracy, data-efficient GNN interatomic potentials, enabling broader application of MLIPs to complex chemical systems.

Active Transfer Bagging: A New Approach for Accelerated Active Learning Acquisition of Data by Combined Transfer Learning and Bagging Based Models

Modern machine learning has achieved remarkable success on many problems, but this success often depends on the existence of large, labeled datasets. While active learning can dramatically reduce labeling cost when annotations are expensive, early performance is frequently dominated by the initial seed set, typically chosen at random. In many applications, however, related or approximate datasets are readily available and can be leveraged to construct a better seed set. We introduce a new method for selecting the seed data set for active learning, Active-Transfer Bagging (ATBagging). ATBagging estimates the informativeness of candidate data point from a Bayesian interpretation of bagged ensemble models by comparing in-bag and out-of-bag predictive distributions from the labeled dataset, yielding an information-gain proxy. To avoid redundant selections, we impose feature-space diversity by sampling a determinantal point process (DPP) whose kernel uses Random Fourier Features and a quality-diversity factorization that incorporates the informativeness scores. This same blended method is used for selection of new data points to collect during the active learning phase. We evaluate ATBagging on four real-world datasets covering both target-transfer and feature-shift scenarios (QM9, ERA5, Forbes 2000, and Beijing PM2.5). Across seed sizes nseed = 10-100, ATBagging improves or ties early active learning and increases area under the learning-curve relative to alternative seed subset selection methodologies in almost all cases, with strongest benefits in low-data regimes. Thus, ATBagging provides a low-cost, high reward means to initiating active learning-based data collection.