Composition of moonmilk deposits located in different zones of the tourist Dolomite Cave of Pozalagua (Karrantza, Basque Country, North of Spain) was established by Raman spectroscopy. The deposits were located in column bases and detached rocks near a gour full of water or a dripping zone. Hydromagnesite (Mg-5(CO3)(4)(OH)(2)center dot 4H(2)O) with a strong Raman band at 1116cm(-1) and weaker ones at 1522vw, 1487vw, 1452vw, 756w, 727w, 466w, 434w, 371w, 327m, 291w, 258w, 247vw and 230 m cm(-1) was found as the main component of the moonmilk. Aragonite is the unique calcium carbonate compound that sometimes composes the moonmilk but always together with the hydromagnesite. Among non-carbonate minerals, some nitrates (nitrocalcite, niter, nitromagnesite, nitratine and gwihabaite) and sulphates (arkanite) were also identified as minor compounds. Most of the deposits were matt white and pasty, but occasionally some samples appear greyish on the surface. In these samples, carbon particles were also found, apart from the above, and Raman shift changes were observed in the hydromagnesite spectra. Apart from the elements involved in the mentioned minerals, Si, Fe, Mn, Zn and Ti were identified by X-ray microfluorescence as trace elements and the results were correlated with mineral compositions found by Raman measurements. Furthermore, quantification of the soluble salts of moonmilk deposits was carried out by ionic chromatography and the results were chemometrically treated to find correlations among soluble ions and the composition of the mineral phases spectroscopically characterised. (c) 2007 Published by Elsevier B.V.