Characterization of organic aerosol across the global remote troposphere: a comparison of ATom measurements and global chemistry models
Authors: Hodzic Alma , Campuzano-Jost Pedro , Bian Huisheng , Chin Mian , Colarco Peter R. , Day Douglas A. , Froyd Karl D. , Heinold Bernd , Jo Duseong S. , Katich Joseph M. , Kodros John K. , Nault Benjamin A. , Pierce Jeffrey R. , Ray Eric , Schacht Jacob , Schill Gregory P. , Schroder Jason C. , Schwarz Joshua P. , Sueper Donna T. , Tegen Ina , Tilmes Simone , Tsigaridis Kostas , Yu Pengfei , Jimenez Jose L. 
Published: April 2020

Abstract. The spatial distribution and properties of submicron organic aerosol (OA)
are among the key sources of uncertainty in our understanding of aerosol
effects on climate. Uncertainties are particularly large over remote regions
of the free troposphere and Southern Ocean, where very few data have been
available and where OA predictions from AeroCom Phase II global models span 2 to 3 orders of magnitude, greatly exceeding the model spread over
source regions. The (nearly) pole-to-pole vertical distribution of
non-refractory aerosols was measured with an aerosol mass spectrometer
onboard the NASA DC-8 aircraft as part of the Atmospheric Tomography (ATom)
mission during the Northern Hemisphere summer (August 2016) and winter
(February 2017). This study presents the first extensive characterization of
OA mass concentrations and their level of oxidation in the remote
atmosphere. OA and sulfate are the major contributors by mass to submicron
aerosols in the remote troposphere, together with sea salt in the marine
boundary layer. Sulfate was dominant in the lower stratosphere. OA
concentrations have a strong seasonal and zonal variability, with the
highest levels measured in the lower troposphere in the summer and over the
regions influenced by biomass burning from Africa (up to 10 µg sm−3). Lower concentrations (∼0.1–0.3 µg sm−3)
are observed in the northern middle and high latitudes and very low
concentrations (<0.1 µg sm−3) in the southern middle and
high latitudes. The ATom dataset is used to evaluate predictions of eight
current global chemistry models that implement a variety of commonly used
representations of OA sources and chemistry, as well as of the AeroCom-II
ensemble. The current model ensemble captures the average vertical and
spatial distribution of measured OA concentrations, and the spread of the
individual models remains within a factor of 5. These results are
significantly improved over the AeroCom-II model ensemble, which shows large
overestimations over these regions. However, some of the improved agreement
with observations occurs for the wrong reasons, as models have the tendency
to greatly overestimate the primary OA fraction and underestimate the
secondary fraction. Measured OA in the remote free troposphere is highly
oxygenated, with organic aerosol to organic carbon (OA ∕ OC) ratios of
∼2.2–2.8, and is 30 %–60 % more oxygenated than in current
models, which can lead to significant errors in OA concentrations. The
model–measurement comparisons presented here support the concept of a more
dynamic OA system as proposed by Hodzic et al. (2016), with enhanced removal
of primary OA and a stronger production of secondary OA in global models
needed to provide better agreement with observations.