source attribution of aerosol size distributions and model evaluation using whistler mountain measurements and geos-chem-tomas simulations
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2016
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Abstract
Remote and free-tropospheric aerosols represent a large fraction of the
climatic influence of aerosols; however, aerosol in these regions is less
characterized than those polluted boundary layers. We evaluate aerosol size
distributions predicted by the GEOS-Chem-TOMAS global chemical transport
model with online aerosol microphysics using measurements from the peak of
Whistler Mountain, British Columbia, Canada
(2182 m a.s.l., hereafter
referred to as Whistler Peak). We evaluate the
model for predictions of aerosol number, size, and composition during periods
of free-tropospheric (FT) and boundary-layer (BL) influence at "coarse"
4° × 5° and "nested"
0.5° × 0.667° resolutions by developing simple FT/BL
filtering techniques. We find that using temperature as a proxy for upslope
flow (BL influence) improved the model–measurement comparisons. The best
threshold temperature was around 2 °C for the coarse simulations and
around 6 °C for the nested simulations, with temperatures warmer
than the threshold indicating boundary-layer air. Additionally, the site was
increasingly likely to be in cloud when the measured relative humidity (RH)
was above 90 %, so we do not compare the modeled and measured size
distributions during these periods. With the inclusion of these temperature
and RH filtering techniques, the model–measurement comparisons improved
significantly. The slope of the regression for N80 (the total number of
particles with particle diameter, Dp, > 80 nm) in the nested
simulations increased from 0.09 to 0.65, R2 increased from 0.04 to 0.46,
and log-mean bias improved from 0.95 to 0.07. We also perform simulations at
the nested resolution without Asian anthropogenic emissions and without
biomass-burning emissions to quantify the contribution of these sources to
aerosols at Whistler Peak (through
comparison with simulations with these emissions on). The long-range
transport of Asian anthropogenic aerosol was found to be significant
throughout all particle number concentrations, and increased N80 by more than
50 %, while decreasing the number of smaller particles because of
suppression of new-particle formation and enhanced coagulation sink.
Similarly, biomass burning influenced Whistler Peak during summer months,
with an increase in N80 exceeding 5000 cm−3. Occasionally, Whistler
Peak experienced N80 > 1000 cm−3 without significant influence from
Asian anthropogenic or biomass-burning aerosol. Air masses were advected at
low elevations through forested valleys during times when temperature and
downwelling insolation were high, ideal conditions for formation of large
sources of low-volatility biogenic secondary organic aerosol (SOA). This
condensable material increased particle growth and hence N80. The low-cost
filtering techniques and source apportionment used in this study can be used
in other global models to give insight into the sources and processes that
shape the aerosol at mountain sites, leading to a better understanding of
mountain meteorology and chemistry.
| Reference Key |
d'andrea2016atmosphericsource
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|---|---|
| Authors | ;S. D. D'Andrea;J. Y. Ng;J. Y. Ng;J. K. Kodros;S. A. Atwood;M. J. Wheeler;A. M. Macdonald;W. R. Leaitch;J. R. Pierce |
| Journal | Journal of agricultural and food chemistry |
| Year | 2016 |
| DOI |
10.5194/acp-16-383-2016
|
| URL | |
| Keywords |
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