Arnaud Demortière

Junhao Cao, Nicolas Folastre, Gozde Oney et al.

This study presents a novel integration of unsupervised learning and decision-making strategies for the advanced analysis of 4D-STEM datasets, with a focus on non-negative matrix factorization (NMF) as the primary clustering method. Our approach introduces a systematic framework to determine the optimal number of components (k) required for robust and interpretable orientation mapping. By leveraging the K-Component Loss method and Image Quality Assessment (IQA) metrics, we effectively balance reconstruction fidelity and model complexity. Additionally, we highlight the critical role of dataset preprocessing in improving clustering stability and accuracy. Furthermore, our spatial weight matrix analysis provides insights into overlapping regions within the dataset by employing threshold-based visualization, facilitating a detailed understanding of cluster interactions. The results demonstrate the potential of combining NMF with advanced IQA metrics and preprocessing techniques for reliable orientation mapping and structural analysis in 4D-STEM datasets, paving the way for future applications in multi-dimensional material characterization.

Fayçal Adrar, Nicolas Folastre, Chloé Pablos et al.

Na-ion batteries have emerged as viable candidates for large-scale energy storage applica- tions due to resource abundance and cost advantages. The constraints imposed on their performance and durability, for instance, by complex phase transformations in positive electrode materials during electrochemical cycling, can be addressed and are thus not detrimental to their development. However, diffusion-limited Na-ion transport can drive spatially heterogeneous phase nucleation and propagation, leading to multiphase coexis- tence and locally non-uniform electrochemical activity, generating complex reaction path- ways that challenge both mechanistic understanding and predictive material optimization. These challenges can be addressed by investigating single-crystalline regions of materials, i.e. down to the scale of individual particles, although such analyses are often constrained by energetically and/or spatially sparse hyperspectral datasets. Here, we developed an AI-driven method to process hyperspectral data under sparse sampling conditions and generate multiphase maps with nanometer-scale resolution over a micrometer-scale field of view. We applied this processing on scanning transmission X-ray microscopy (STXM) data to determine the distribution and coexistence of phases in individual particles of NaxV2(PO4)2F3 cathode materials, at different states of charge. The methodology relies on a workflow which combines a Gaussian mixture variational autoencoder (GMVAE) algorithm with the Pearson corre- lation coefficient to identify the sodium content and map their spatial distribution. Our approach reveals nanoscale phase heterogeneity and evolution within individual particles, and improves the reliability of phase detection by identifying ambiguity zones, false assign- ments, and transition phases localized at grain boundaries.

Antoine Bottenmuller, Florent Magaud, Arnaud Demortière et al.

With the aim of estimating the abundance map from observations only, linear unmixing approaches are not always suitable to spectral images, especially when the number of bands is too small or when the spectra of the observed data are too correlated. To address this issue in the general case, we present a novel approach which provides an adapted spatial density function based on any arbitrary linear classifier. A robust mathematical formulation for computing the Euclidean distance to polyhedral sets is presented, along with an efficient algorithm that provides the exact minimum-norm point in a polyhedron. An empirical evaluation on the widely-used Samson hyperspectral dataset demonstrates that the proposed method surpasses state-of-the-art approaches in reconstructing abundance maps. Furthermore, its application to spectral images of a Lithium-ion battery, incompatible with linear unmixing models, validates the method's generality and effectiveness.