Mardochée Réveil, PhD

Rapid progress in aberration corrected electron microscopy necessitates development of robust methods for the identification of phases, ferroic variants, and other pertinent aspects of materials structure from imaging data. While unsupervised methods for clustering and classification are widely used for these tasks, their performance can be sensitive to hyperparameter selection in the analysis workflow. In this study, we explore the effects of descriptors and hyperparameters on the capability of unsupervised ML methods to distill local structural information, exemplified by discovery of polarization and lattice distortion in Sm doped BiFeO3 (BFO) thin films. We demonstrate that a reward-driven approach can be used to optimize these key hyperparameters across the full workflow, where rewards were designed to reflect domain wall continuity and straightness, ensuring that the analysis aligns with the material's physical behavior. This approach allows us to discover local descriptors that are best aligned with the specific physical behavior, providing insight into the fundamental physics of materials. We further extend the reward driven workflows to disentangle structural factors of variation via optimized variational autoencoder (VAE). Finally, the importance of well-defined rewards was explored as a quantifiable measure of success of the workflow.

Synchrotron radiation sources play a crucial role in fields such as materials science, biology, and chemistry. The beamline, a key subsystem of the synchrotron, modulates and directs the radiation to the sample for analysis. However, the alignment of beamlines is a complex and time-consuming process, primarily carried out manually by experienced engineers. Even minor misalignments in optical components can significantly affect the beam's properties, leading to suboptimal experimental outcomes. Current automated methods, such as bayesian optimization (BO) and reinforcement learning (RL), although these methods enhance performance, limitations remain. The relationship between the current and target beam properties, crucial for determining the adjustment, is not fully considered. Additionally, the physical characteristics of optical elements are overlooked, such as the need to adjust specific devices to control the output beam's spot size or position. This paper addresses the alignment of beamlines by modeling it as a Markov Decision Process (MDP) and training an intelligent agent using RL. The agent calculates adjustment values based on the current and target beam states, executes actions, and iterates until optimal parameters are achieved. A policy network with action attention is designed to improve decision-making by considering both state differences and the impact of optical components. Experiments on two simulated beamlines demonstrate that our algorithm outperforms existing methods, with ablation studies highlighting the effectiveness of the action attention-based policy network.

Reconstructing the physical complexity of many-body dynamical systems can be challenging. Starting from the trajectories of their constitutive units (raw data), typical approaches require selecting appropriate descriptors to convert them into time-series, which are then analyzed to extract interpretable information. However, identifying the most effective descriptor is often non-trivial. Here, we report a data-driven approach to compare the efficiency of various descriptors in extracting information from noisy trajectories and translating it into physically relevant insights. As a prototypical system with non-trivial internal complexity, we analyze molecular dynamics trajectories of an atomistic system where ice and water coexist in equilibrium near the solid/liquid transition temperature. We compare general and specific descriptors often used in aqueous systems: number of neighbors, molecular velocities, Smooth Overlap of Atomic Positions (SOAP), Local Environments and Neighbors Shuffling (LENS), Orientational Tetrahedral Order, and distance from the fifth neighbor ($d_5$). Using Onion Clustering -- an efficient unsupervised method for single-point time-series analysis -- we assess the maximum extractable information for each descriptor and rank them via a high-dimensional metric. Our results show that advanced descriptors like SOAP and LENS outperform classical ones due to higher signal-to-noise ratios. Nonetheless, even simple descriptors can rival or exceed advanced ones after local signal denoising. For example, $d_5$, initially among the weakest, becomes the most effective at resolving the system's non-local dynamical complexity after denoising. This work highlights the critical role of noise in information extraction from molecular trajectories and offers a data-driven approach to identify optimal descriptors for systems with characteristic internal complexity.