Two-year measurements of Black Carbon properties at the high-altitude mountain site of Pic du Midi Observatory in the French Pyrenees
Authors: Tinorua Sarah , Denjean Cyrielle , Nabat Pierre , Bourrianne Thierry , Pont Véronique , Gheusi François , Leclerc Emmanuel 
Published: April 2023

Abstract. Black Carbon containing particles (BC) are strong light absorbers, causing substantial radiative heating of the atmosphere. The climate-relevant properties of BC are poorly constrained in high-elevation mountain regions, where numerous complex interactions between BC, radiation, clouds and snow have important climate implications. This study presents two-year measurements of BC microphysical and optical properties at the research station of Pic du Midi (PDM), a high-altitude observatory located at 2877 m above sea level in the French Pyrenees. Among the worldwide existing long-term monitoring sites, PDM has experiences limited influence of the planetary boundary layer (PBL), making it an appropriate site for characterizing free tropospheric (FT) BC. The classification of the dominant aerosol type using the spectral optical properties of the aerosols indicates that BC was the predominant absorption component of aerosols at PDM and controlled the variation of Single Scattering Albedo (SSA) throughout the two years. Single-particle soot photometer (SP2) measurements showed a mean mass concentrations of BC (MBC) of 35 ng m−3 and a relatively constant BC core mass-equivalent diameter of around 180 nm, which are typical values for remote mountain sites. Combining the MBC with in situ absorption measurements yielded a BC mass absorption coefficient (MACBC) of 9.8 ± 2.7 m2 g−1 at 880 nm, which corresponds to an absorption enhancement (Eabs) of 2.4 compared to that of bare BC particles with equal BC core size distribution. A significant reduction of the ratio ∆BC / ∆CO when precipitation occurred along the air mass transport suggests wet removal of BC. However we found that the wet removal process did not affect the size of BC, resulting in unchanged Eabs . We observed a large seasonal contrast in BC properties with higher MBC and Eabs in summer than winter. In winter a strong diurnal variability of MBC (Eabs) with higher (lower) values in the middle of the day was linked to the injection of BC originating from the PBL. During summer in contrast, MBC showed no diurnal variation was rather constant despite more frequent PBL-conditions, implying that MBC fluctuations were rather dominated by regional and long-range transport in the FT. A body of evidence suggests that biomass burning emissions effectively altered the concentration and optical properties of BC at PDM, leading to higher Eabs in summer compared to winter. The diurnal pattern of Eabs in summer was opposite to that observed in winter with maximum values of 2.9 observed at noon. We suggest that this daily variation results from photochemical processing driving BC mixing state rather than a change in BC emission source. Such direct two-year observations of BC properties provide quantitative constraints for both regional and global climate models and have the potential to close the gap between model predicted and observed effects of BC on regional radiation budget and climate. The results demonstrates the complex influence of BC emission sources, transport pathways, atmospheric dynamics and chemical reactivity in driving the light absorption of BC.