Reflections from the 2024 Large Language Model (LLM) Hackathon for Applications in Materials Science and Chemistry

Here, we present the outcomes from the second Large Language Model (LLM) Hackathon for Applications in Materials Science and Chemistry, which engaged participants across global hybrid locations, resulting in 34 team submissions. The submissions spanned seven key application areas and demonstrated the diverse utility of LLMs for applications in (1) molecular and material property prediction; (2) molecular and material design; (3) automation and novel interfaces; (4) scientific communication and education; (5) research data management and automation; (6) hypothesis generation and evaluation; and (7) knowledge extraction and reasoning from scientific literature. Each team submission is presented in a summary table with links to the code and as brief papers in the appendix. Beyond team results, we discuss the hackathon event and its hybrid format, which included physical hubs in Toronto, Montreal, San Francisco, Berlin, Lausanne, and Tokyo, alongside a global online hub to enable local and virtual collaboration. Overall, the event highlighted significant improvements in LLM capabilities since the previous year's hackathon, suggesting continued expansion of LLMs for applications in materials science and chemistry research. These outcomes demonstrate the dual utility of LLMs as both multipurpose models for diverse machine learning tasks and platforms for rapid prototyping custom applications in scientific research.

Machine Learning-Based Reward-Driven Tuning of Scanning Probe Microscopy: Towards Fully Automated Microscopy

Since the dawn of scanning probe microscopy (SPM), tapping or intermittent contact mode has been one of the most widely used imaging modes. Manual optimization of tapping mode not only takes a lot of instrument and operator time, but also often leads to frequent probe and sample damage, poor image quality and reproducibility issues for new types of samples or inexperienced users. Despite wide use, optimization of tapping mode imaging is an extremely hard problem, ill-suited to either classical control methods or machine learning. Here we introduce a reward-driven workflow to automate the optimization of SPM in the tapping mode. The reward function is defined based on multiple channels with physical and empirical knowledge of good scans encoded, representing a sample-agnostic measure of image quality and imitating the decision-making logic employed by human operators. This automated workflow gives optimal scanning parameters for different probes and samples and gives high-quality SPM images consistently in the attractive mode. This study broadens the application and accessibility of SPM and opens the door for fully automated SPM.

Invariant Discovery of Features Across Multiple Length Scales: Applications in Microscopy and Autonomous Materials Characterization

Physical imaging is a foundational characterization method in areas from condensed matter physics and chemistry to astronomy and spans length scales from atomic to universe. Images encapsulate crucial data regarding atomic bonding, materials microstructures, and dynamic phenomena such as microstructural evolution and turbulence, among other phenomena. The challenge lies in effectively extracting and interpreting this information. Variational Autoencoders (VAEs) have emerged as powerful tools for identifying underlying factors of variation in image data, providing a systematic approach to distilling meaningful patterns from complex datasets. However, a significant hurdle in their application is the definition and selection of appropriate descriptors reflecting local structure. Here we introduce the scale-invariant VAE approach (SI-VAE) based on the progressive training of the VAE with the descriptors sampled at different length scales. The SI-VAE allows the discovery of the length scale dependent factors of variation in the system. Here, we illustrate this approach using the ferroelectric domain images and generalize it to the movies of the electron-beam induced phenomena in graphene and topography evolution across combinatorial libraries. This approach can further be used to initialize the decision making in automated experiments including structure-property discovery and can be applied across a broad range of imaging methods. This approach is universal and can be applied to any spatially resolved data including both experimental imaging studies and simulations, and can be particularly useful for exploration of phenomena such as turbulence, scale-invariant transformation fronts, etc.

Integration of Scanning Probe Microscope with High-Performance Computing: fixed-policy and reward-driven workflows implementation

The rapid development of computation power and machine learning algorithms has paved the way for automating scientific discovery with a scanning probe microscope (SPM). The key elements towards operationalization of automated SPM are the interface to enable SPM control from Python codes, availability of high computing power, and development of workflows for scientific discovery. Here we build a Python interface library that enables controlling an SPM from either a local computer or a remote high-performance computer (HPC), which satisfies the high computation power need of machine learning algorithms in autonomous workflows. We further introduce a general platform to abstract the operations of SPM in scientific discovery into fixed-policy or reward-driven workflows. Our work provides a full infrastructure to build automated SPM workflows for both routine operations and autonomous scientific discovery with machine learning.

Multimodal Co-orchestration for Exploring Structure-Property Relationships in Combinatorial Libraries via Multi-Task Bayesian Optimization

The rapid growth of automated and autonomous instrumentations brings forth an opportunity for the co-orchestration of multimodal tools, equipped with multiple sequential detection methods, or several characterization tools to explore identical samples. This can be exemplified by the combinatorial libraries that can be explored in multiple locations by multiple tools simultaneously, or downstream characterization in automated synthesis systems. In the co-orchestration approaches, information gained in one modality should accelerate the discovery of other modalities. Correspondingly, the orchestrating agent should select the measurement modality based on the anticipated knowledge gain and measurement cost. Here, we propose and implement a co-orchestration approach for conducting measurements with complex observables such as spectra or images. The method relies on combining dimensionality reduction by variational autoencoders with representation learning for control over the latent space structure, and integrated into iterative workflow via multi-task Gaussian Processes (GP). This approach further allows for the native incorporation of the system's physics via a probabilistic model as a mean function of the GP. We illustrated this method for different modalities of piezoresponse force microscopy and micro-Raman on combinatorial $Sm-BiFeO_3$ library. However, the proposed framework is general and can be extended to multiple measurement modalities and arbitrary dimensionality of measured signals. The analysis code that supports the funding is publicly available at https://github.com/Slautin/2024_Co-orchestration.

Human-in-the-loop: The future of Machine Learning in Automated Electron Microscopy

Machine learning methods are progressively gaining acceptance in the electron microscopy community for de-noising, semantic segmentation, and dimensionality reduction of data post-acquisition. The introduction of the APIs by major instrument manufacturers now allows the deployment of ML workflows in microscopes, not only for data analytics but also for real-time decision-making and feedback for microscope operation. However, the number of use cases for real-time ML remains remarkably small. Here, we discuss some considerations in designing ML-based active experiments and pose that the likely strategy for the next several years will be human-in-the-loop automated experiments (hAE). In this paradigm, the ML learning agent directly controls beam position and image and spectroscopy acquisition functions, and human operator monitors experiment progression in real- and feature space of the system and tunes the policies of the ML agent to steer the experiment towards specific objectives.

EGraFFBench: Evaluation of Equivariant Graph Neural Network Force Fields for Atomistic Simulations

Equivariant graph neural networks force fields (EGraFFs) have shown great promise in modelling complex interactions in atomic systems by exploiting the graphs' inherent symmetries. Recent works have led to a surge in the development of novel architectures that incorporate equivariance-based inductive biases alongside architectural innovations like graph transformers and message passing to model atomic interactions. However, thorough evaluations of these deploying EGraFFs for the downstream task of real-world atomistic simulations, is lacking. To this end, here we perform a systematic benchmarking of 6 EGraFF algorithms (NequIP, Allegro, BOTNet, MACE, Equiformer, TorchMDNet), with the aim of understanding their capabilities and limitations for realistic atomistic simulations. In addition to our thorough evaluation and analysis on eight existing datasets based on the benchmarking literature, we release two new benchmark datasets, propose four new metrics, and three new challenging tasks. The new datasets and tasks evaluate the performance of EGraFF to out-of-distribution data, in terms of different crystal structures, temperatures, and new molecules. Interestingly, evaluation of the EGraFF models based on dynamic simulations reveals that having a lower error on energy or force does not guarantee stable or reliable simulation or faithful replication of the atomic structures. Moreover, we find that no model clearly outperforms other models on all datasets and tasks. Importantly, we show that the performance of all the models on out-of-distribution datasets is unreliable, pointing to the need for the development of a foundation model for force fields that can be used in real-world simulations. In summary, this work establishes a rigorous framework for evaluating machine learning force fields in the context of atomic simulations and points to open research challenges within this domain.

Discovering mesoscopic descriptions of collective movement with neural stochastic modelling

Collective motion is an ubiquitous phenomenon in nature, inspiring engineers, physicists and mathematicians to develop mathematical models and bio-inspired designs. Collective motion at small to medium group sizes ($\sim$10-1000 individuals, also called the `mesoscale'), can show nontrivial features due to stochasticity. Therefore, characterizing both the deterministic and stochastic aspects of the dynamics is crucial in the study of mesoscale collective phenomena. Here, we use a physics-inspired, neural-network based approach to characterize the stochastic group dynamics of interacting individuals, through a stochastic differential equation (SDE) that governs the collective dynamics of the group. We apply this technique on both synthetic and real-world datasets, and identify the deterministic and stochastic aspects of the dynamics using drift and diffusion fields, enabling us to make novel inferences about the nature of order in these systems.