Global simulations of nitrate and ammonium aerosols and their radiative effects

Xu, Li; Penner, Joyce E.

doi:10.5194/acp-12-9479-2012

Cited by 183 publications

(263 citation statements)

References 101 publications

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“…Xu and Penner, 2012) as can be seen 15 from Table 7. While the total NO x emissions (except for lightning as discussed above) are very similar to other recent studies, the dry and wet deposition rates are about a factor of three lower.…”

Section: No X Budgetsupporting

confidence: 68%

“…This is due to the parameterisation of the heterogeneous uptake of HNO 3 on seasalt and dust aerosols, which removes HNO 3 from the system and does not allow for re-evaporation from the aerosol or droplet phase. The sensitivity run no_het_HNO3 yields dry and wet deposition rates of nitrogen which are very close to Xu and Penner (2012) and in the range of other model studies (Liao et al, 2004;Rodriguez and Dabdub, 2004;Feng and Penner, 2007).…”

Section: No X Budgetmentioning

confidence: 48%

See 1 more Smart Citation

The Chemistry Climate Model ECHAM6.3-HAM2.3-MOZ1.0

Schultz¹,

Stadtler²,

Schröder³

et al. 2017

Geosci. Model Dev. Discuss.

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Abstract. The chemistry climate model ECHAM-HAMMOZ contains a detailed representation of tropospheric and stratospheric reactive chemistry and state-of-the-art parametrisations of aerorols using either a modal scheme (M7) or a bin scheme (SALSA). This article describes and evaluates the model version ECHAM6.3-HAM2.3-MOZ1.0 with a focus on the tropospheric gas-phase chemistry. A ten-year model simulation was performed to test the stability of the model and provide data for Global budgets of ozone, hydroxide (OH), nitrogen oxides (NO x ), aerosols, clouds, and radiation are analyzed and compared 10 to the literature. ECHAM-HAMMOZ performs well in many aspects. However, in the base simulation, lightning NO x emissions are very low, and the impact of the heterogeneous reaction of HNO 3 on dust and seasalt aerosol is too strong. Sensitivity simulations with increased lightning NO x or modified heterogeneous chemistry deteriorate the comparison with observations and yield excessively large ozone budget terms and too much OH. We hypothesize that this is an impact of potential issues with tropical convection in the ECHAM model.

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Section: No X Budgetsupporting

confidence: 68%

Section: No X Budgetmentioning

confidence: 48%

The Chemistry Climate Model ECHAM6.3-HAM2.3-MOZ1.0

Schultz¹,

Stadtler²,

Schröder³

et al. 2017

Geosci. Model Dev. Discuss.

View full text Add to dashboard Cite

show abstract

“…Nitric acid was chosen as it is abundant in the atmosphere with concentrations up to several parts per billion, and its effect on cloud droplet formation is modelled in several publications (e.g. Kulmala et al, 1993;Laaksonen et al, 1998;Nenes et al, 2002;Romakkaniemi et al, 2005;Makkonen et al, 2012;Xu and Penner, 2012). HNO 3 has a Henry law coefficient of 2.1 × 10 5 mol kg −1 atm −1 at room temperature.…”

Section: Introductionmentioning

confidence: 99%

Ammonium nitrate evaporation and nitric acid condensation in DMT CCN counters

et al. 2014

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Abstract. The effect of inorganic semivolatile aerosol compounds on the cloud condensation nucleus (CCN) activity of aerosol particles was studied by using a computational model for a DMT-CCN counter, a cloud parcel model for condensation kinetics and experiments to quantify the modelled results. Concentrations of water vapour and semivolatiles as well as aerosol trajectories in the CCN column were calculated by a computational fluid dynamics model. These trajectories and vapour concentrations were then used as an input for the cloud parcel model to simulate mass transfer kinetics of water and semivolatiles between aerosol particles and the gas phase.Two different questions were studied: (1) how big a fraction of semivolatiles is evaporated from particles after entering but before particle activation in the DMT-CCN counter? (2) How much can the CCN activity be increased due to condensation of semivolatiles prior to the maximum water supersaturation in the case of high semivolatile concentration in the gas phase?Both experimental and modelling results show that the evaporation of ammonia and nitric acid from ammonium nitrate particles causes a 10 to 15 nm decrease to the critical particle size in supersaturations between 0.1 % and 0.7 %. On the other hand, the modelling results also show that condensation of nitric acid or similar vapour can increase the CCN activity of nonvolatile aerosol particles, but a very high gas phase concentration (as compared to typical ambient conditions) would be needed. Overall, it is more likely that the CCN activity of semivolatile aerosol is underestimated than overestimated in the measurements conducted in ambient conditions.

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“…This inaccuracy need not be related to the model assumptions and simplifications, as there are other likely causes. The amount of nitric acid dissolving into the particle phase is highly dependent on particle pH, and thus the ability to accurately predict particulate nitrate in such sulfate-rich regions is dependent also on the amount of sulfuric acid vs. ammonia (e.g., Xu and Penner, 2012). When comparing the model values to the observations, one also needs to consider the representativeness of the monitoring site in relation to the model resolution.…”

Section: Global Model Implementation and Experimental Set-upmentioning

confidence: 99%

Size-resolved simulations of the aerosol inorganic composition with the new hybrid dissolution solver HyDiS-1.0: description, evaluation and first global modelling results

et al. 2016

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Abstract. The dissolution of semi-volatile inorganic gases such as ammonia and nitric acid into the aerosol aqueous phase has an important influence on the composition, hygroscopic properties, and size distribution of atmospheric aerosol particles. The representation of dissolution in global models is challenging due to inherent issues of numerical stability and computational expense. For this reason, simplified approaches are often taken, with many models treating dissolution as an equilibrium process. In this paper we describe the new dissolution solver HyDiS-1.0, which was developed for the global size-resolved simulation of aerosol inorganic composition. The solver applies a hybrid approach, which allows for some particle size classes to establish instantaneous gas-particle equilibrium, whereas others are treated time dependently (or dynamically). Numerical accuracy at a competitive computational expense is achieved by using several tailored numerical formalisms and decision criteria, such as for the time-and size-dependent choice between the equilibrium and dynamic approaches. The new hybrid solver is shown to have numerical stability across a wide range of numerical stiffness conditions encountered within the atmosphere. For ammonia and nitric acid, HyDiS-1.0 is found to be in excellent agreement with a fully dynamic benchmark solver. In the presence of sea salt aerosol, a somewhat larger bias is found under highly polluted conditions if hydrochloric acid is represented as a third semi-volatile species. We present first results of the solver's implementation into a global aerosol microphysics and chemistry transport model. We find that (1) the new solver predicts surface concentrations of nitrate and ammonium in reasonable agreement with observations over Europe, the USA, and East Asia, (2) models that assume gas-particle equilibrium will not capture the partitioning of nitric acid and ammonia into Aitken-mode-sized particles, and thus may be missing an important pathway through which secondary particles may grow to radiation-and cloudinteracting size, and (3) the new hybrid solver's computational expense is modest, at around 10 % of total computation time in these simulations.

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Global simulations of nitrate and ammonium aerosols and their radiative effects

Cited by 183 publications

References 101 publications

The Chemistry Climate Model ECHAM6.3-HAM2.3-MOZ1.0

The Chemistry Climate Model ECHAM6.3-HAM2.3-MOZ1.0

Ammonium nitrate evaporation and nitric acid condensation in DMT CCN counters

Size-resolved simulations of the aerosol inorganic composition with the new hybrid dissolution solver HyDiS-1.0: description, evaluation and first global modelling results

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