The formation of new aerosol particles in the atmosphere is a key process influencing the aerosol number concentration as well as the climate, in particular in the free troposphere (FT) where the newly formed particles directly influence cloud formation. However, free tropospheric new particle formation (NPF) is poorly documented due to logistic limitations and complex atmospheric dynamics around high altitude stations that make the observation of this day-time process challenging. Recent improvements in measurement techniques make now possible the detection of neutral clusters down to ~ 1 nm sizes, which opens new horizons in our understanding of the nucleation process. Indeed, only the charged fraction of clusters has been reported in the upper troposphere up to now. Here we report observations of charged and neutral clusters (1 to 2.5 nm mobility diameter) during day-time free tropospheric conditions at the altitude site of Puy de Dôme (1465 m a.s.l.), central France, between 10 and 29 February 2012. Our findings demonstrate that in the free troposphere, the formation of 1.5 nm neutral clusters is about 40 times higher than the one of ionic clusters during NPF events, indicating that they dominate in the nucleation process. We also observe that the total cluster concentration increases by a factor of 5.5 during NPF events compared to the other days, which was not clearly observed for the charged cluster population in the past. In the FT, the nucleation process does not seem to be sulphuric acid-limited, as previously suggested, and could be promoted by the transport of pollutants to the upper troposphere.