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Two important processes at organic-organic interfaces in which defects dramatically impact chemistry are energy transfer between surface functional groups of carbon dots and singlet/triplet exciton interconversion at grain boundaries of organic solids. These systems possess a diversity in chemical structures of which only a small subset, dependent on preparation method and surface treatment, may play an outsize role in determining the overall dynamic behavior. The expected outcomes of NSF CAFF are transformative knowledge about how to exploit defects through imaging at atomic, nano- and microscales; spectroscopic insight across multiple time domains; and partnership with theory. Innovations include new data-driven algorithms and modular instrumentation that are crucial for broadening access and advancing physical chemistry.