global evaluation of ammonia bidirectional exchange and livestock diurnal variation schemes
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2015
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Abstract
Bidirectional air–surface exchange of ammonia (NH3) has been neglected in
many air quality models. In this study, we implement the bidirectional
exchange of NH3 in the GEOS-Chem global chemical transport model. We also
introduce an updated diurnal variability scheme for NH3 livestock
emissions and evaluate the recently developed MASAGE_NH3 bottom-up
inventory. While updated diurnal variability improves comparison of
modeled-to-hourly in situ measurements in the southeastern USA, NH3
concentrations decrease throughout the globe, up to 17 ppb in India and
southeastern China, with corresponding decreases in aerosol nitrate by up to
7 μg m−3. The ammonium (NH4+) soil pool in the
bidirectional exchange model largely extends the NH3 lifetime in the
atmosphere. Including bidirectional exchange generally increases NH3
gross emissions (7.1 %) and surface concentrations (up to 3.9 ppb)
throughout the globe in July, except in India and southeastern China. In
April and October, it decreases NH3 gross emissions in the Northern
Hemisphere (e.g., 43.6 % in April in China) and increases NH3 gross
emissions in the Southern Hemisphere. Bidirectional exchange does not
largely impact NH4+ wet deposition overall. While bidirectional exchange
is fundamentally a better representation of NH3 emissions from
fertilizers, emissions from primary sources are still underestimated and thus
significant model biases remain when compared to in situ measurements in the
USA. The adjoint of bidirectional exchange has also been developed for the
GEOS-Chem model and is used to investigate the sensitivity of NH3
concentrations with respect to soil pH and fertilizer application rate. This
study thus lays the groundwork for future inverse modeling studies to more
directly constrain these physical processes rather than tuning bulk
unidirectional NH3 emissions.
| Reference Key |
zhu2015atmosphericglobal
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|---|---|
| Authors | ;L. Zhu;D. Henze;J. Bash;G.-R. Jeong;K. Cady-Pereira;M. Shephard;M. Luo;F. Paulot;S. Capps |
| Journal | Journal of agricultural and food chemistry |
| Year | 2015 |
| DOI |
10.5194/acp-15-12823-2015
|
| URL | |
| Keywords |
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