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Synthetic organic dyes were extensively used by artists in the first half of the 20th century, knowingly or otherwise. This included Andy Warhol and his À la Recherche du Shoe Perdu (c. 1955), a major portfolio of hand-colored prints, a copy of which resides in the collection of The Museum of Modern Art (MoMA). Warhol and his friends were known to use Dr. Ph. Martin’s Synchromatic Transparent Water Colors to bring these prints to life. A historical set of Synchromatic Transparent Watercolors were initially investigated by UV-visible spectroscopy, and samples from the historic set were also characterized by µ-Fourier transform infrared spectroscopy for fingerprint identification. To better elucidate the nature of the mixtures present, thin-layer chromatography was coupled with surface-enhanced Raman spectroscopy to separate the components of all colorants in the set. The dyes decisively identified include Acid Red 73, Acid Red 87, Acid Red 17, Acid Red 103, Basic Red 1, Acid Orange 7, Acid Yellow 23, Acid Green 1, Basic Green 4, Acid Blue 3, Acid Blue 93, Basic Violet 3, Basic Violet 10, Basic Violet 17, and Acid Black 2. Overall, Acid Blue 3, along with Acid Orange 7 and Acid Black 2, were found in the greatest number of dyes in the Dr. Ph. Martin’s set. Data from the historic set was subsequently used for direct comparison with reflectance spectra from the Warhol portfolio using principal component analysis. Microfade testing on a Synchromatic Transparent Watercolors brochure was also conducted to identify fugitive colorants, the results of which were extrapolated to each of the prints in the Warhol portfolio. The analysis provided further insight into the dyes used in À la Recherche du Shoe Perdu and confirmed the extreme light sensitivity of some colorants and the fastness of others. Full article