Two-year intercomparison of three methods for measuring black carbon concentration at a high-altitude research station in Europe

Abstract. Black carbon (BC) is one of the most important climate forcer with severe health effects. Large uncertainties in radiative forcing estimation and health impact assessment arise from the fact that there is no standardized method to measure BC mass concentration. This study presents a two-year comparison of three state-of-the-art BC measurement techniques at the high-altitude research station Pic du Midi located in the French Pyrenees at an altitude of 2877 m above sea level. A recently upgraded aethalometer AE33, a thermal-optical analyzer Sunset and a single-particle soot photometer SP2 were deployed to measure simultaneously the mass concentration of equivalent black carbon (M_eBC), elemental carbon (M_EC) and refractory black carbon (M_rBC), respectively. Significant deviations in the response of the instruments were observed. All techniques responded to seasonal variations of the atmospheric changes in BC levels and exhibited good correlation during the whole study period. This indicates that the different instruments quantified the same particle type, despite the fact that they are based on different physical principles. However the slopes and correlation coefficients varied between instrument pairs. The largest biases were observed for the AE33 with M_eBC values that were around 2 times greater than M_rBC and M_EC values. The principal reasons of such large discrepancy was explained by the too low MAC and C values recommended by the AE33 manufacturer and applied to the absorption coefficients measured by the AE33. In addition, the long-range transport of dust particles at PDM in spring caused significant increases in the bias between AE33 and SP2 by up to a factor 8. The Sunset M_EC measurements agreed within around 17 % with the SP2 M_rBC values. The largest overestimations of M_EC were observed when the total carbon concentration were below 25 µgC cm⁻² , which is probably linked to the incorrect determination of the OC-EC split point. Another cause of the discrepancy between instruments was found to be the limited detection range of the SP2, which did not allow the total detection of fine rBC particles. The procedure used to estimate the missing mass fraction of rBC not covered by the measurement range of the SP2 was found to be critical. We found that a time-dependent correction based on fitting the observed rBC size distribution with a multimodal lognormal distribution are needed to accurately estimate M_rBC over a larger size range.