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Airborne and ground-based differential optical absorption spectroscopy observations have been carried out at the volcano Nyiragongo (Democratic Republic of Congo) to measure SO2 and bromine monoxide (BrO) in the plume in March 2004 and June 2007, respectively. Additionally filter pack and multicomponent gas analyzer system (Multi-GAS) measurements were carried out in June 2007. Our measurements provide valuable information on the chemical composition of the volcanic plume emitted from the lava lake of Nyiragongo. The main interest of this study has been to investigate for the first time the bromine emission flux of Nyiragongo (a rift volcano) and the BrO formation in its volcanic plume. Measurement data and results from a numerical model of the evolution of BrO in Nyiragongo volcanic plume are compared with earlier studies of the volcanic plume of Etna (Italy). Even though the bromine flux from Nyiragongo (2.6 t/d) is slightly greater than that from Etna (1.9 t/d), the BrO/SO2 ratio (maximum 7 × 10-5) is smaller than in the plume of Etna (maximum 2.1 × 10-4). A one-dimensional photochemical model to investigate halogen chemistry in the volcanic plumes of Etna and Nyiragongo was initialized using data from Multi-GAS and filter pack measurements. Model runs showed that the differences in the composition of volcanic volatiles led to a smaller fraction of total bromine being present as BrO in the Nyiragongo plume and to a smaller BrO/SO2 ratio.