Micro-Raman spectroscopy was applied in characterisation of inks and pigments used in the text, illuminations and miniatures of two old-Slavonic manuscripts: Vrutok four gospels (13th-14th centuries) and Benche four gospels (16th century). They were written in old-Slavonic language with old Cyrillic alphabet. Both were decorated with ornaments in so called Balkan style characterised with intertwined rings and floral motifs. Only four colours/pigments were used in the simple miniature and ornaments in Vrutok book: orpiment, vermilion, organo-copper complex and mixed ink. Much richer palette of pigments was revealed in the Benche book: calcite, gypsum, lead white, yellow ochre, pararealgar/realgar, vermilion, red lead, red ocra, organo-copper complex, malachite, indigo, iron gall ink, carbon black and pure metallic gold. The use of pigments in ornaments compared with miniatures is somewhat different in Benche book, suggesting that either handwriting and ornamenting on one side and miniatures, on the other, were done by different persons/painters or depiction of sacral themes of the miniatures canonically required the use of more expensive/elaborate pigments.Micro-Raman spectroscopy allowed in situ, non-destructive, rapid and unambiguous identification of the majority of pigments used in the text, ornamentations and miniatures in the Vrutok and Benche four gospels. In case of uncertainty in identification of pigments, scanning electron microscopy-energy dispersive X-ray analysis was applied.

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Micro-Raman spectroscopy, pyrolysis/gas chromatography-mass spectrometry (Py/GC/MS) and gas chromatography-mass spectrometry (CG/MS) were applied for the characterization of pigments and binders used in the wall paintings ascribed to the works of the prominent 19 th century Macedonian iconographer, Dicho Zograph. Among numerous works attributed to him, wall paintings from three churches in the Western part of the Republic of Macedonia have been selected for pigment and binder analysis.A rich palette of pigments, both natural/mineral and synthetic ones, were identified by micro-Raman spectroscopy. Organic material analysis evidenced the use of mixtures of proteinaceous materials (mainly animal glue and egg) with linseed oil and pine resin, while saccharide materials were excluded.

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