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The Peleș National Museum in Sinaia, Romania, includes within its collection of musical instruments a unique harpsichord of the Taskin workshop. The instrument is representative of the eighteenth century French harpsichords, finished in 1772 by Taskin Pascal, a master instrument-maker of his time. This paper presents the results of a comprehensive diagnostic investigation carried out on the exterior decoration of the harpsichord, by means of multiple non-invasive and micro-invasive analytical techniques: multispectral imaging, X-ray fluorescence (XRF) spectroscopy, laser-induced breakdown spectroscopy (LIBS), Fourier transform infrared spectroscopy (FTIR), and optical microscopy (OM). Imaging investigation highlighted various past interventions and restorations—fillings, consolidation and chromatic reintegration of the paint layer, as well as some interesting details related to the preparatory layer and on the painting technique. Results of the elemental analysis indicated that a rich color palette was used for the luxurious decorations: vermilion for most of the red areas, lead white, a copper-based pigment for the blue and violet hues, along with Prussian blue, chromium oxides for the green tones and possibly emerald green, and iron oxides for the red, yellow and ochre tones. FTIR analysis highlighted the existence of two-layers ground based on the first layer of chalk and animal glue, covered by a second oil-bound layer of lead white. Metal soaps, gypsum, barium sulfate as well as an intermediate sizing layer based on shellac were also identified. Examination of samples' cross-sections revealed a rich stratigraphy, up to ten layers being highlighted for samples taken from the case sides' painting. The presence of two gold foils on the gilded areas, one at the top and the other within the intermediate layers, provides clear evidence of later interventions. The corroborated results offer valuable physico-chemical insights on the complex history of this prestigious harpsichord with remarkable aesthetic and historical value, as well as key information for its most suitable restoration approach. [ABSTRACT FROM AUTHOR]