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CAFF will develop transformative experimental and computational tools to understand intrinsically disordered systems and apply them to molecular materials that defy conventional approaches. Our team is uniquely suited to apprehend the multi-dimensional parameter space of intrinsically disordered systems at the cutting edge of interpretation and acquisition with spatially and temporally resolved chemical information. CAFF will cultivate new spectroscopic imaging capabilities by integrating computer vision concepts to achieve transformative temporal, spatial, and spectral resolution to confront blind spots in ensemble averaging. We will develop “smart” microscopy strategies where real-time analysis drives data collection to anticipate emergent function. In order to leverage the broad capabilities within CAFF to generate definitive structure-function relationships, we will develop transformational data-driven strategies that integrate datasets from multiple sub-ensemble measurements with state-of-the-art theoretical tools from electronic structure theory, statistical physics, and dynamics.