Detection of mixing and precipitation scavenging effects on biomass
burning aerosols using total water heavy isotope ratios during ORACLES
Abstract
The prevalence of mixing vs. precipitation processes in biomass burning
aerosol (BBA) laden air over the southeast Atlantic is assessed during
three intensive observation periods during the NASA ORACLES
(ObseRvations of Aerosols above CLouds and their intEractionS) campaign.
Air in the lower free troposphere (FT) and marine boundary layer (MBL)
are treated as separate analyses, although connections are made where
relevant. The study, centering on aircraft in-situ measurements of total
water heavy isotope ratios, has two main objectives. The first is to
gauge whether the atmospheric hydrology, and in particular
precipitation, can be constrained primarily through visual assessment of
the aircraft isotope ratio data plotted against total water
concentration, similarly to several previous studies. However,
regression of the data onto a simple model of convective detrainment is
also used and alludes to the possibility of a precipitation data product
derived from isotope ratios. The second objective is to connect
variations in aerosol concentrations to the hydrology as diagnosed by
the isotope ratio measurements, and determine whether aerosol variations
are attributable to wet scavenging. First, joint water concentration (q)
and H2O/HDO isotope measurements (δD) in the lower FT are combined with
satellite and MERRA-2 data into simple analytical models to constrain
hydrologic histories of BBA-laden air originating over Africa and
flowing over the southeast Atlantic. We find that even simple models are
capable of detecting and constraining the primary processes at play.
Further, a strong correlation between isotopic evidence of precipitation
in lower FT air masses and an in-situ indicator of wet scavenging of
black carbon – the ratio of black carbon to carbon monoxide (BC/CO) –
is shown. In comparison, the correlation between BC/CO and the water
concentration itself is low. Since wet scavenging is the primary removal
mechanism of black carbon, these findings suggest that isotope
measurements could support studies constraining the lifetime of black
carbon in the FT. Next, the ability of measurements interpreted with
simple analytical models in (q, δD) space to distinguish cloud-top
entrainment vs. precipitation signals in the MBL is tested. This proves
more difficult than the lower FT analysis since signals are smaller. We
find that the largest obstacle to this goal is the (q, δD) values of the
entrained airmass at cloud-top. We also compare cloud condensation
nuclei (CCN) concentrations in the sub-cloud layer to the isotopic
measurements. In 2016 and 2018 IOPs, lower CCN concentrations coincide
with isotope ratio evidence of precipitation, indicating aerosol
scavenging. However, a more complex model simulating water, isotope
ratios, and aerosols would be necessary to achieve more definitive
conclusions. For the 2017 IOP, with the highest sub-cloud CCN
concentrations, there is no connection between precipitation signals and
CCN concentrations.