Correlative X-ray and electron tomography for scale-bridging, quantitative analysis of complex, hierarchical particle systems

Abstract: This study presents a comprehensive workflow for investigating particulate materials through combined 360{\deg} electron tomography (ET), nano-computed X-ray tomography (nanoCT), and micro-computed X-ray tomography (microCT), alongside a versatile sample preparation routine. The workflow enables the investigation of size, morphology, and pore systems across multiple scales, from individual particles to large hierarchical structures. A customized tapered sample shape is fabricated using focused ion beam milling with the aim to optimize each imaging technique's field of view, facilitating high-resolution analysis of small volumes containing single particles, while also allowing for large-scale studies of thousands of particles for statistical relevance. By correlating data from same locations in different imaging modalities, the approach enhances the precision of quantitative analyses. The study highlights the importance of cross-scale, correlative three-dimensional microscopy for a comprehensive understanding of complex hierarchical materials. Precise data registration, segmentation using machine learning, and multimodal imaging techniques are crucial for unlocking insights into process-structure-property relationships and thus to optimize functional, hierarchical materials.