The attractiveness of natural and cultured pearls is related, in part, to their colour. Raman spectroscopy was applied to natural and cultured pearls and the shells from 23 species of pearl producing molluscs, thus covering the majority of the natural and cultured pearls and their host animals found in the market today, in order to better understand their colouration and eventually to be able to identify the host animal. Pigments with a polyenic chain were identified in samples from 18 species. The vast majority were found to be a mixture of partially methylated polyenes, similar to those observed in octocorals. Samples with a similar colour but from different animal species can be sometimes related to a significantly different mixtures of such pigments. Only natural pearls from Pinna nobilis were found to be coloured by carotenoids. Raman spectra of other pigments were also observed on samples from four species, possibly linked with pigments from the porphyrin group.

The present study applied Laser Ablation-Inductively Coupled Plasma-Mass Spectrometry (LA-ICP-MS) on a large number of natural and cultured pearls from saltwater and freshwater environments, which revealed that freshwater (natural and cultured) pearls contain relatively higher quantities of manganese (Mn) and barium (Ba) and lower sodium (Na), magnesium (Mg) and strontium (Sr) than saltwater (natural and cultured) pearls. A few correlations between the host animal’s species and chemical elements were found; some samples from Pinctada maxima (P. maxima) are the only studied saltwater samples with 55Mn >20 ppmw, while some P. radiata are the only studied saltwater samples with 24Mg <65 ppmw and some of the P. imbricata are the only studied saltwater samples with 137Ba >4.5 ppmw. X-ray luminescence reactions of the studied samples has confirmed a correlation between its yellow-green intensity and manganese content in aragonite, where the higher Mn2+ content, the more intense the yellow-green luminescence becomes. Luminescence intensity in some cases is lower even if manganese increases, either because of pigments or because of manganese self-quenching. X-ray luminescence can be applied in most cases to separate saltwater from freshwater samples; only samples with low manganese content (55Mn <50 ppmw) might be challenging to identify. One of the studied natural freshwater pearls contained vaterite sections which react by turning orange under X-ray due to a different coordination of Mn2+ in vaterite than that in aragonite.