Development of an improved two-sphere integration technique for quantifying black carbon concentrations in the atmosphere and seasonal snow

<jats:p>Abstract. An improved two-sphere integration (TSI) technique has been developed to quantify black carbon (BC) concentrations in the atmosphere and seasonal snow. The major advantage of this system is that it combines two distinct integrated spheres to reduce the scattering effect due to light-absorbing particles and thus provides accurate determinations of total light absorption from BC collected on Nuclepore filters. The TSI technique can be calibrated using a series of 15 filter samples of standard fullerene soot. This technique quantifies the mass of BC by separating the spectrally resolved total light absorption into BC and non-BC fractions. To assess the accuracy of the improved system, an empirical procedure for measuring BC concentrations with a two-step thermal–optical method is also applied. Laboratory results indicate that the BC concentrations determined using the TSI technique and theoretical calculations are well correlated (R2=0.99), whereas the thermal–optical method underestimates BC concentrations by 35 %–45 % compared to that measured by the TSI technique. Assessments of the two methods for atmospheric and snow samples revealed excellent agreement, with least-squares regression lines with slopes of 1.72 (r2=0.67) and 0.84 (r2=0.93), respectively. However, the TSI technique is more accurate in quantifications of BC concentrations in both the atmosphere and seasonal snow, with an overall lower uncertainty. Using the improved TSI technique, we find that light absorption at a wavelength of 550 nm due to BC plays a dominant role relative to non-BC light absorption in both the atmosphere (62.76 %–91.84 % of total light absorption) and seasonal snow (43.11 %–88.56 %) over northern China. </jats:p>