Assessment of Easily Accessible Spectroscopic Techniques Coupled with Multivariate Analysis for the Qualitative Characterization and Differentiation of Earth Pigments of Various Provenance

Ioana Maria Cortea · Luminița Ghervase · Roxana N. Radvan · George Calin Seritan

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Cultural Heritage Materials Analysis Mineralogy and Gemology Studies Spectroscopy and Chemometric Analyses

Abstract

Natural minerals and earths with coloring properties have been widely used as artistic pigments since prehistoric times. Despite being extensively studied, the complex chemistry of earth pigments is still unsatisfactory described with respect to their mineralogical and structural variability and origin. In this study, a large group of earth pigments from various geographical locations was investigated using easily accessible spectroscopic techniques and multivariate analysis with the aim to identify distinctive mineralogical and chemical characteristics of natural pigment sources. Portable X-ray fluorescence (p-XRF), Fourier transform infrared spectroscopy (FTIR) and fiberoptic Raman spectroscopy were used for the elemental, molecular and structural characterization of the investigated pigments. Diagnostic spectral features and chemical patterns (fingerprints) were identified and discussed with respect to their geological sources. Due to the occurrence of similar accompanying minerals, it was observed that the differentiation of red and yellow ochers is more challenging compared to green, brown and black pigments. However, for some of the investigated pigments, the presence of certain accessory minerals and/or of certain chemical patterns can have diagnostic value. Principal component analysis (PCA) of the FTIR and XRF data matrices showed promising results in terms of geological attribution, highlighting a promising tool for provenance research. The results of the study demonstrate the potential benefits of this rapid and nondestructive approach for the characterization and differentiation of earth pigments with similar hues coming from different geological sources.

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References

2009Engraved ochres from the Middle Stone Age levels at Blombos Cave, South Africa 2007Heated goethite and natural hematite: Can Raman spectroscopy be used to differentiate them?2003Clay and iron oxide pigments in the history of painting 2000Ochre-differentiation through micro-Raman and micro-FTIR spectroscopies: application on wall paintings at Meteora and Mount Athos, Greece 2008Raman identification of natural red to yellow pigments: ochre and iron‐containing ores 2008Pigment Compendium 2002Systematic Pigment Use in the Middle Pleistocene of South‐Central Africa 2011Reflection infrared spectroscopy for the non-invasive in situ study of artists’ pigments

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