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JOURNAL OF GEOPHYSICAL RESEARCH,
VOL. 108, NO. D12,
4353,
doi:10.1029/2002JD002890,
2003
Moment-based simulation of microphysical properties of sulfate aerosols in the eastern United States: Model description, evaluation,
and regional analysis
Shaocai Yu
Nicholas School of the Environmental and Earth Sciences, Duke University, Durham, North Carolina, USA
Prasad S. Kasibhatla
Nicholas School of the Environmental and Earth Sciences, Duke University, Durham, North Carolina, USA
Douglas L. Wright
Nicholas School of the Environmental and Earth Sciences, Duke University, Durham, North Carolina, USA
Stephen E. Schwartz
Atmospheric Sciences Division, Brookhaven National Laboratory, Upton, New York, USA
Robert McGraw
Atmospheric Sciences Division, Brookhaven National Laboratory, Upton, New York, USA
Aijun Deng
Department of Meteorology, Pennsylvania State University, University Park, Pennsylvania, USA
Abstract
A six-moment microphysics module for sulfate aerosols based on the quadrature method of moments has been incorporated in a
host 3-D regional model, the Multiscale Air Quality Simulation Platform. Model performance was examined and evaluated by comparison
with in situ observations over the eastern United States for a 40-day period from 19 July to 28 August 1995. The model generally
reproduces the spatial patterns (sulfate mixing ratios and wet deposition) over the eastern United States and time series
variations of sulfate mass concentrations. The model successfully captured the observed size distribution in the accumulation
mode (radius 0.1–0.5 μm), in which the sulfate is predominately located, while underestimating the nucleation and coarse modes
on the basis of the size distributions retrieved from the modeled six moments at the Great Smoky Mountains (GSM). This is
consistent with better model performance on the effective radius (ratio of third to second moment, important for light scattering)
than on number-mean and mass-mean radii. However, the model did not predict some of the moments well, especially the higher
moments and during the dust events. Aerosol components other than sulfate such as dust and organics appear to have contributed
substantially to the observed aerosol loading at GSM. The model underpredicted sulfate mixing ratios by 13% with about 50%
of observations simulated to within a factor of 2. One of the reasons for this underestimation may be overprediction of sulfate
wet deposition. Sulfate mass concentrations and number concentrations were high in the source-rich Ohio River valley, but
number concentrations were also high over the mid-Atlantic coast (New Jersey area). Most (77%) sulfate amount was below 2.6
km, whereas most sulfate number (>52%) was above 2.6 km except over Ohio River valley (41%). These results demonstrate the
accuracy, utility, practicality, and efficiency of moment-based methods for representing aerosol microphysical processes in
large-scale chemical transport models.
Received 28
August
2002;
accepted 19
February
2003;
published 19
June
2003.
Index Terms: 0305 Atmospheric Composition and Structure: Aerosols and particles (0345, 4801); 0345 Atmospheric Composition and Structure: Pollution—urban and regional (0305); 0365 Atmospheric Composition and Structure: Troposphere—composition and chemistry; 0368 Atmospheric Composition and Structure: Troposphere—constituent transport and chemistry.
Read Full Article (file size: 2111630 bytes) Cited by
Citation: Yu, S., P. S. Kasibhatla, D. L. Wright, S. E. Schwartz, R. McGraw, and A. Deng
(2003),
Moment-based simulation of microphysical properties of sulfate aerosols in the eastern United States: Model description, evaluation,
and regional analysis,
J. Geophys. Res.,
108(D12),
4353,
doi:10.1029/2002JD002890.
Copyright 2003 by the American Geophysical Union.
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