Mihail Bogojeski

Parastoo Semnani, Mihail Bogojeski, Florian Bley et al.

The successful application of machine learning (ML) in catalyst design relies on high-quality and diverse data to ensure effective generalization to novel compositions, thereby aiding in catalyst discovery. However, due to complex interactions, catalyst design has long relied on trial-and-error, a costly and labor-intensive process leading to scarce data that is heavily biased towards undesired, low-yield catalysts. Despite the rise of ML in this field, most efforts have not focused on dealing with the challenges presented by such experimental data. To address these challenges, we introduce a robust machine learning and explainable AI (XAI) framework to accurately classify the catalytic yield of various compositions and identify the contributions of individual components. This framework combines a series of ML practices designed to handle the scarcity and imbalance of catalyst data. We apply the framework to classify the yield of various catalyst compositions in oxidative methane coupling, and use it to evaluate the performance of a range of ML models: tree-based models, logistic regression, support vector machines, and neural networks. These experiments demonstrate that the methods used in our framework lead to a significant improvement in the performance of all but one of the evaluated models. Additionally, the decision-making process of each ML model is analyzed by identifying the most important features for predicting catalyst performance using XAI methods. Our analysis found that XAI methods, providing class-aware explanations, such as Layer-wise Relevance Propagation, identified key components that contribute specifically to high-yield catalysts. These findings align with chemical intuition and existing literature, reinforcing their validity. We believe that such insights can assist chemists in the development and identification of novel catalysts with superior performance.

Sasho Nedelkoski, Mihail Bogojeski, Odej Kao

Data often are formed of multiple modalities, which jointly describe the observed phenomena. Modeling the joint distribution of multimodal data requires larger expressive power to capture high-level concepts and provide better data representations. However, multimodal generative models based on variational inference are limited due to the lack of flexibility of the approximate posterior, which is obtained by searching within a known parametric family of distributions. We introduce a method that improves the representational capacity of multimodal variational methods using normalizing flows. It approximates the joint posterior with a simple parametric distribution and subsequently transforms into a more complex one. Through several experiments, we demonstrate that the model improves on state-of-the-art multimodal methods based on variational inference on various computer vision tasks such as colorization, edge and mask detection, and weakly supervised learning. We also show that learning more powerful approximate joint distributions improves the quality of the generated samples. The code of our model is publicly available at https://github.com/SashoNedelkoski/BPFDMVM.

Mihail Bogojeski, Muhammad R. Hasyim, Leslie Vogt-Maranto et al.

Machine-learning interatomic potentials (MLIPs) have enabled molecular dynamics at near ab initio accuracy, yet remain limited to energies and forces by construction, leaving electronic observables such as dipole moments and polarizabilities inaccessible. We introduce DenSNet, a density-first approach to machine-learned electronic structure that learns the Hohenberg--Kohn map from nuclear configurations to the ground-state electron density. Our approach employs an SE(3)-equivariant neural network to predict density coefficients of a flexible atom-centered Gaussian basis, combined with a $Δ$-learning strategy that uses superposed atomic densities as a prior to accelerate training. A second equivariant network then maps the predicted density to the total energy, providing a unified framework for molecular dynamics and electronic structure. We validate DenSNet on ethanol, ethanethiol, and resorcinol, where infrared spectra from machine-learned trajectories show excellent agreement with experimental gas-phase measurements. To test scalability, we train on polythiophene oligomers with 1--6 monomers and extrapolate to chains of up to 12 monomers, generating stable long-time trajectories whose infrared spectra agree with reference density functional theory calculations. Here, we show that reinstating the electron density as the central learned quantity opens a practical route to transferable prediction of spectroscopic and electronic observables in large-scale molecular simulations.

Oliver T. Unke, Mihail Bogojeski, Michael Gastegger et al.

Machine learning has enabled the prediction of quantum chemical properties with high accuracy and efficiency, allowing to bypass computationally costly ab initio calculations. Instead of training on a fixed set of properties, more recent approaches attempt to learn the electronic wavefunction (or density) as a central quantity of atomistic systems, from which all other observables can be derived. This is complicated by the fact that wavefunctions transform non-trivially under molecular rotations, which makes them a challenging prediction target. To solve this issue, we introduce general SE(3)-equivariant operations and building blocks for constructing deep learning architectures for geometric point cloud data and apply them to reconstruct wavefunctions of atomistic systems with unprecedented accuracy. Our model achieves speedups of over three orders of magnitude compared to ab initio methods and reduces prediction errors by up to two orders of magnitude compared to the previous state-of-the-art. This accuracy makes it possible to derive properties such as energies and forces directly from the wavefunction in an end-to-end manner. We demonstrate the potential of our approach in a transfer learning application, where a model trained on low accuracy reference wavefunctions implicitly learns to correct for electronic many-body interactions from observables computed at a higher level of theory. Such machine-learned wavefunction surrogates pave the way towards novel semi-empirical methods, offering resolution at an electronic level while drastically decreasing computational cost. Additionally, the predicted wavefunctions can serve as initial guess in conventional ab initio methods, decreasing the number of iterations required to arrive at a converged solution, thus leading to significant speedups without any loss of accuracy or robustness.

Mihail Bogojeski, Simeon Sauer, Franziska Horn et al.

Accurately predicting industrial aging processes makes it possible to schedule maintenance events further in advance, ensuring a cost-efficient and reliable operation of the plant. So far, these degradation processes were usually described by mechanistic or simple empirical prediction models. In this paper, we evaluate a wider range of data-driven models, comparing some traditional stateless models (linear and kernel ridge regression, feed-forward neural networks) to more complex recurrent neural networks (echo state networks and LSTMs). We first examine how much historical data is needed to train each of the models on a synthetic dataset with known dynamics. Next, the models are tested on real-world data from a large scale chemical plant. Our results show that recurrent models produce near perfect predictions when trained on larger datasets, and maintain a good performance even when trained on smaller datasets with domain shifts, while the simpler models only performed comparably on the smaller datasets.