The effect of nitric acid uptake on the deliquescence and efflorescence of binary ammoniated salts in the upper troposphere

2002 ◽  
Vol 29 (10) ◽  
pp. 126-1-126-4 ◽  
Author(s):  
Jin-Sheng Lin ◽  
Azadeh Tabazadeh
Author(s):  
Eric Scheuer ◽  
Jack E. Dibb ◽  
Cynthia Twohy ◽  
David C. Rogers ◽  
Andrew J. Heymsfield ◽  
...  
Keyword(s):  

2021 ◽  
Author(s):  
Nana wei ◽  
eloise a. marais ◽  
paul o. wennberg ◽  
hannah m. allen ◽  
john d. crounse ◽  
...  

<p>Reactive nitrogen in the upper troposphere (~8-12 km) impacts global climate, air quality and the oxidizing capacity of the whole troposphere. Here we use aircraft observations from instruments onboard the NASA DC8 aircraft for campaigns from 1997 (SONEX) to the recent ATom campaign (2016-2018) and the MOZAIC commercial aircraft campaign (2003-2005) to address uncertainties in the dynamics of reactive nitrogen (NO<sub>y</sub> = NO<sub>x</sub> + NO<sub>x</sub> reservoir compounds) in the global upper troposphere (UT). Our initial analysis of the DC8 aircraft observations is consistent with previous work in that PAN is the dominant NO<sub>y</sub> component (average: 43%; range: 40-60%), followed by NO<sub>x </sub>(on average, 21%), with smaller contributions (on average, 3.5-12.5%) from pernitric acid (HNO<sub>4</sub>), organonitrate (RONO<sub>2</sub>) and nitric acid (HNO<sub>3</sub>). We go on to compare multiyear mean NO<sub>y</sub> from MOZAIC to the combination of all NASA DC8 campaigns to determine whether we can build a near-global climatology of NO<sub>y</sub> and its components to compare to GEOS-Chem to assess our understanding of these very important atmospheric components.</p>


2012 ◽  
Vol 12 (2) ◽  
pp. 653-667 ◽  
Author(s):  
B. H. Henderson ◽  
R. W. Pinder ◽  
J. Crooks ◽  
R. C. Cohen ◽  
A. G. Carlton ◽  
...  

Abstract. Tropospheric ozone is the third strongest greenhouse gas, and has the highest uncertainty in radiative forcing of the top five greenhouse gases. Throughout the troposphere, ozone is produced by radical oxidation of nitrogen oxides (NOx = NO + NO2). In the upper troposphere (8–10 km), current chemical transport models under-estimate nitrogen dioxide (NO2) observations. Improvements to simulated NOx production from lightning have increased NO2 predictions, but the predictions in the upper troposphere remain biased low. The upper troposphere has low temperatures (T < 250 K) that increase the uncertainty of many important chemical reaction rates. This study constrains uncertain reaction rates by combining model predictions with measurements from the Intercontinental Chemical Transport Experiment-North America observational campaign. The results show that the nitric acid formation rate, which is the dominant sink of NO2 and radicals, is currently over-estimated by 22% in the upper troposphere. The results from this study suggest that the temperature sensitivity of nitric acid formation is lower than currently recommended. Since the formation of nitric acid removes nitrogen dioxide and radicals that drive the production of ozone, the revised reaction rate will affect ozone concentrations in upper troposphere impacting climate and air quality in the lower troposphere.


2021 ◽  
Vol 21 (20) ◽  
pp. 15901-15927
Author(s):  
Anthony C. Jones ◽  
Adrian Hill ◽  
Samuel Remy ◽  
N. Luke Abraham ◽  
Mohit Dalvi ◽  
...  

Abstract. Ammonium nitrate is a major aerosol constituent over many land regions and contributes to air pollution episodes, ecosystem destruction, regional haze, and aerosol-induced climate forcing. Many climate models that represent ammonium nitrate assume that the ammonium–sulfate–nitrate chemistry reaches thermodynamic equilibrium instantaneously without considering kinetic limitations on condensation rates. The Met Office's Unified Model (UM) is employed to investigate the sensitivity of ammonium nitrate concentrations to the nitric acid uptake coefficient (γ) in a newly developed nitrate scheme in which first-order condensation theory is utilised to limit the rate at which thermodynamic equilibrium is attained. Two values of γ representing fast (γ=0.193) and slow (γ=0.001) uptake rates are tested in 20-year global UM integrations. The global burden of nitrate associated with ammonium in the “fast” simulation (0.11 Tg[N]) is twice as great as in the “slow” simulation (0.05 Tg[N]), while the top-of-the-atmosphere radiative impact of representing nitrate is −0.19 W m−2 in the fast simulation and −0.07 W m−2 in the slow simulation. In general, the fast simulation exhibits better spatial correlation with observed nitrate concentrations, while the slow simulation better resolves the magnitude of concentrations. Local near-surface nitrate concentrations are found to be highly correlated with seasonal ammonia emissions, suggesting that ammonia is the predominant limiting factor controlling nitrate prevalence. This study highlights the high sensitivity of ammonium nitrate concentrations to nitric acid uptake rates and provides a novel mechanism for reducing nitrate concentration biases in climate model simulations. The new UM nitrate scheme represents a step change in aerosol modelling capability in the UK across weather and climate timescales.


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