Chromatic Signatures and Comprehensive Archaeometric Investigations of Prehistoric Ochre from Southern Romania

This study investigates the composition, morphology and cultural significance of red pigment traces identified on bone pointed tools discovered in the Chalcolithic tell settlement of Pietrele–Măgura Gorgana, attributed to the Kodjadermen–Gumelnița–Karanovo VI cultural complex (4600–4250 BC). The observed use-wear patterns are consistent with repeated contact with soft, non-abrasive materials, including hide working, pigment application on leather or other organic surfaces, fiber manipulation, and perforation of soft substrates. Use-wear analysis revealed polished and flattened distal ends, compatible with repeated use on soft, non-abrasive materials, such as hide, leather, fiber, or other organic substrates. The possibility of pigment application directly on skin, in a practice analogous to tattooing, as previously published, cannot be excluded but remains speculative in the absence of experimental reference data or residue evidence specifically linked to such use. An associated ceramic container was tentatively interpreted as a possible vessel for ochre preparation, suggesting local processing of the pigment. The artifacts were investigated using multi-analytical archaeometric methods: SEM-EDS, AFM, TEM, FTIR, Raman, TGA, CLSM and pseudo-color image segmentation and 3D rendering of porosity distribution. The results consistently identified an iron oxide-based pigment, dominated by hematite and/or goethite, specific to ochre. Pigment particles (50–300 nm) form a well-defined superficial layer on the bone substrate, without Fe–Ca reactions at the interface. The simultaneous presence of Ca, P, Si, Mg and K indicates a silicate matrix with an apatite component, compatible with local and poorly purified raw materials. CIELAB colorimetric analyses revealed significant chromatic variability, suggesting the use of hematite-rich pigments and possible thermal transformations of goethite. The results contribute to the understanding of the pigment technologies of the Chalcolithic communities of the Lower Danube.