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The intensive variables of dacitic–rhyodacitic magmas prior to four large Plinian eruptions of Santorini Volcano over the last 200 kyr (Minoan, Cape Riva, Lower Pumice 2 and Lower Pumice 1) were determined by combining crystallization experiments with study of the natural products, including the volatile contents of melt inclusions trapped in phenocrysts. Phase equilibria of the silicic magmas were determined at pressures of 1, 2 and 4 kbar, temperatures of 850–900°C, fluid (H2O + CO2)-saturation, XH2O [= molar H2O/(H2O + CO2)] between 0·6 and 1 (melt H2O contents of 2–10 wt %), and redox conditions of FMQ (fayalite–magnetite–quartz buffer) or NNO + 1 (where NNO is Ni–NiO buffer). Experiments were generally successful in reproducing the phenocryst assemblage of the natural products. The phase relationships vary significantly among the investigated compositions, revealing a sensitivity to small variations in whole-rock compositions. Our results show that the pre-eruptive storage conditions of the four silicic magmas were all very similar. The magmas were stored at T = 850–900°C and P ≥ 2 kbar, under moderately reduced conditions (ΔNNO = −0·9 to −0·1), and were poor in fluorine (∼500–800 ppm) and sulphur (≤100 ppm), but rich in water and chlorine (5–6 wt % and 2500–3500 ppm, respectively). In all cases, the melts were slightly undersaturated with respect to H2O, but most probably saturated with respect to H2O + Cl ± CO2 and a brine. The Santorini magma plumbing system appears to be dominated by a large, long-lived (≥200 kyr) predominantly silicic magma storage region situated at ≥8 km depth, from which crystal-poor melt batches were extracted during the largest caldera-forming eruptions of the volcanic system. [ABSTRACT FROM PUBLISHER]