Detection of dilution due to turbulent mixing vs. precipitation scavenging effects on biomass burning aerosol concentrations using stable water isotope ratios during ORACLES

Abstract. The interaction between biomass burning aerosols and clouds remains challenging to accurately determine, in part because of difficulties using direct observations to account for influences on aerosol concentrations from precipitation scavenging and dilution due to air mass mixing and separating those signals from source contributions. The prevalence of mixing versus precipitation processes in air laden with biomass burning aerosol (BBA) in the southeast Atlantic lower free troposphere (FT) and marine boundary layer (MBL) is assessed during three observation periods (September 2016, August 2017, and October 2018) during the NASA ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) campaign. Significant sources of BBAs over the African continent combined with regional circulation patterns result in BBA-laden air flowing from the continent over the southeast Atlantic in the lower FT, then subsiding onto the semi-permanent stratocumulus cloud deck, and entraining into the MBL. This study is broken into two parts, first analyzing hydrologic histories of the BBA air in the lower FT and then carrying out a similar assessment in the underlying MBL. Both analyses leverage joint measurements of water concentration and its heavy isotope ratio, interpreted in the previously established (q, δD) phase space framework. For the lower-FT analysis, in situ observations (water concentration, water isotope ratios) in the lower FT are combined with satellite and Modern-Era Retrospective analysis for Research and Applications, Version 2 (MERRA-2), global reanalysis data into simple analytical models to constrain hydrologic histories. We find that even simple models are capable of detecting and constraining the primary processes at play, e.g., distinguishing air masses that experienced moist convection and precipitation (likely over the continent) from those that underwent dry convection and turbulent mixing. Regression of the aircraft data onto a simple model of convective detrainment is used to develop a metric of total precipitation for the in situ measurements and then compared to an aerosol metric of black carbon scavenging also derived from the in situ measurements (the ratio of black carbon to carbon monoxide, BC/CO). There is a strong correlation between the two, suggesting black carbon scavenging has been detected and partially quantified, if only in a relative manner. In comparison, weak correlation is found between BC/CO and the total water concentration itself. The above method is expanded to test for entrainment and precipitation influences on BBA concentrations in the MBL. This is more difficult than the FT analysis since signals are subtle and limited by imperfect knowledge of the water and isotope ratios of the entrained air mass at cloud top. For some of the MBLs observed during 2016 and 2018, lower cloud condensation nuclei (CCN) concentrations occur in the sub-cloud layer coincident with isotopic evidence of precipitation, indicating aerosol scavenging, but more complex models are needed to produce definitive conclusions. For the 2017 observation period, with the highest sub-cloud CCN concentrations, there is no connection between precipitation signals and CCN concentrations, likely indicating the importance of different geographic sampling and air mass history in that year. Nonetheless, these findings along with the FT analysis suggest that utilizing isotope ratio signals may be an aid in addressing cloud–aerosol challenges. Especially for the FT case, these findings support the pursuit of more complex models combined with targeted in situ data to constrain BC scavenging coefficients in a manner which can guide model parameterizations, leading to improvements in the accuracy of simulated BC concentrations and lifetimes in climate models.