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We describe analytical details and uncertainty evaluation of a simple technique for the measurement of the carbon isotopic composition of CO in volcanic plumes. Data collected at Solfatara and Vulcano, where plumes are fed by fumaroles which are accessible for direct sampling, were first used to validate the technique. For both volcanoes, the plume-derived carbon isotopic compositions are in good agreement with the fumarolic compositions, thus providing confidence on the method, and allowing its application at volcanoes where the volcanic component is inaccessible to direct sampling. As a notable example, we applied the same method to Mount Etna where we derived a δC of volcanic CO between −0.9 ± 0.27‰ and −1.41 ± 0.27‰ (Bocca Nuova and Voragine craters). The comparison of our measurements to data reported in previous work highlights a temporal trend of systematic increase of δC values of Etna CO from ~ −4‰, in the 1970's and the 1980's, to ~ −1‰ at the present time (2009). This shift toward more positive δC values matches a concurrent change in magma composition and an increase in the eruption frequency and energy. We discuss such variations in terms of two possible processes: magma carbonate assimilation and carbon isotopic fractionation due to magma degassing along the Etna plumbing system. Finally, our results highlight potential of systematic measurements of the carbon isotopic composition of the CO emitted by volcanic plumes for a better understanding of volcanic processes and for improved surveillance of volcanic activity. [ABSTRACT FROM AUTHOR]