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Life on Earth depends on photosynthesis. Photosynthetic systems evolved early in Earth history and have been stable for 2.5 billion years, providing prima facie evidence for the significance of pigments in plant functions. Photosynthetic pigments fill multiple roles from increasing the range of energy captured for photosynthesis to protective functions. Given the importance of pigments to leaf functioning, greater effort is needed to determine whether individual pigments can be identified and quantified in vivo using high fidelity spectroscopy. We review recent advances in detecting plant pigments at the leaf level and discuss successes and reasons why challenges remain for robust remote observation and quantification. New methods to identify and quantify individual pigments in the presence of overlapping absorption features would provide a major advance in understanding their biological functions, quantifying net carbon exchange, and identifying plant stresses.