Observation-Based Constraints on Modeled Aerosol Surface Area:
Implications for Heterogeneous Chemistry
Abstract
Heterogeneous reactions occurring at the surface of atmospheric aerosol
particles regulate the production and lifetime of a wide array of
atmospheric gases. Aerosol surface area plays a critical role in setting
the rate of heterogeneous reactions in atmospheric chemistry. Despite
the central role for aerosol surface area, there are few assessments of
the accuracy of aerosol surface area concentrations in regional and
global models. In this study, we compare aerosol surface area
concentrations in the EPA’s CMAQ (Community Multiscale Air Quality)
model with commensurate observations from the 2011 NASA flight-based
DISCOVER-AQ (Deriving Information on Surface Conditions from COlumn and
VERtically Resolved Observations Relevant to Air Quality) campaign. The
study region for the 2011 DISCOVER-AQ campaign focused primarily on the
Baltimore and Washington, DC region. Dry aerosol surface area was
measured aboard the NASA P-3B aircraft using a combination of a Scanning
Mobility Particle Sizer (SMPS), Aerodynamic Particle Sizer (APS), and
Ultra-High Sensitivity Aerosol Spectrometer (UHSAS). In this study, we
focus on the continuous 1s UHSAS measurements in size range of
60-1000nm, as it captures the majority of the dry surface area
distribution. Over the course of 13 flight campaigns, we show strong
agreement between measured and modeled aerosol number concentration
(CMAQ Number/UHSAS Number= 0.88). In contrast, the total surface area
showed a larger discrepancy (CMAQ surface area/UHSAS surface area =
0.44). We hypothesize that the emissions and chemistry in CMAQ relating
to the production and loss of each moment play a large part in the
model/measurement discrepancy. Despite the disagreement, this analysis
suggests that modeled aerosol surface area is accurate to within a
factor of two, highlighting that uncertainty in the rate of
heterogeneous reactions is largely driven by uncertainty in the reactive
uptake coefficients. We would like to thank the DISCOVER-AQ NASA Langley
Aerosol Research Group Experiment (LARGE) research team, including
Richard Moore, Bruce Anderson, Andreas Beyersdorf, Luke Ziemba, Lee
Thornhill, and Edward Winstead for the use of their data in this study.