Volcanic eruptions caused major weather and climatic changes on timescales ranging from hours to centuries in the past. Volcanic particles are injected in the atmosphere both as primary particles rapidly deposited due to their large sizes on time scales of minutes to a few weeks in the troposphere, and secondary particles mainly derived from the oxidation of sulfur dioxide. These particles are responsible for the atmospheric cooling observed at both regional and global scales following large volcanic eruptions. However, large condensational sinks due to preexisting particles within the plume, and unknown nucleation mechanisms under these circumstances make the assumption of new secondary particle formation still uncertain because the phenomenon has never been observed in a volcanic plume. In this work, we report the first observation of nucleation and new secondary particle formation events in a volcanic plume. These measurements were performed at the puy de Dôme atmospheric research station in central France during the Eyjafjallajokull volcano eruption in Spring 2010. We show that the nucleation is indeed linked to exceptionally high concentrations of sulfuric acid and present an unusual high particle formation rate. In addition we demonstrate that the binary H 2 SO 4 − H 2 O nucleation scheme, as it is usually considered in modeling studies, underestimates by 7 to 8 orders of magnitude the observed particle formation rate and, therefore, should not be applied in tropospheric conditions. These results may help to revisit all past simulations of the impact of volcanic eruptions on climate.secondary aerosols | volcanic sulfur | nanoparticles V olcanic eruptions and their impact on climate have been extensively investigated in geological archives such as sediments (1), ice cores (2-5), and through modeling studies (6, 7) but processes taking place in the volcanic plume have rarely been directly observed. The sulfur dioxide emitted in large amounts during explosive volcanic eruptions (8) can be oxidized to sulfuric acid, thus many authors suspect that the formed sulfuric acid gives rise to the formation of new secondary particle from binary homogeneous nucleation mechanism (1, 9-12). Those new particles can then affect the atmospheric radiative balance both directly and indirectly because they can act as cloud condensation nuclei (CCN) (13). This leads to a cooling effect, which is on a time scale from months to years, depending on the location of the eruption and the height at which volcanic gases were emitted.The Eyjafjallajokull volcano located in the south of Iceland [63°38′ N, 19°36′ W, summit 1,660 m above sea level (asl)] erupted on March 20, 2010. A major outbreak of the central crater under the covering ice cap followed on April 14, 2010 (Institute of Earth Sciences, 2010). A large volcanic plume composed of ashes and gases rose up to the tropopause level (approximately 10 km) for days and were observed by satellite and ground-based remote sensing instruments. The volcanic plume reached European altitude s...