Condensable vapour concentrations and aerosol formation rates in toluene oxidation experiments using a least-squares aerosol dynamics model

2004 ◽  
Vol 35 ◽  
pp. 355-368
Author(s):  
T. Petäjä ◽  
K.E.J. Lehtinen ◽  
Ü. Rannik ◽  
M. Kulmala
Atmosphere ◽  
2020 ◽  
Vol 11 (9) ◽  
pp. 1004
Author(s):  
Hyo-Jung Lee ◽  
Hyun-Young Jo ◽  
Chang-Keun Song ◽  
Yu-Jin Jo ◽  
Shin-Young Park ◽  
...  

A numerical sensitivity study on secondary organic aerosol formation has been carried out by employing the WRF-Chem (Weather Research and Forecasting model coupled with Chemistry). Two secondary organic aerosol formation modules, the Modal Aerosol Dynamics model for Europe/Volatility Basis Set (MADE/VBS) and the Modal Aerosol Dynamics model for Europe/Secondary Organic Aerosol Model (MADE/SORGAM) were employed in the WRF-Chem model, and surface PM2.5 (particulate matter less than 2.5 μm in size) mass concentration and the composition of its relevant chemical sources, i.e., SO42−, NO3−, NH4+, and organic carbon (OC) were simulated during the Korea-United States Air Quality (KORUS-AQ) campaign period (1 May to 12 June 2016). We classified the KORUS-AQ period into two cases, the stagnant period (16–21 May) which was dominated by local emission and the long-range transport period (25–31 May) which was affected by transport from the leeward direction, and focused on the differences in OC secondary aerosol formation between two modules over Northeast Asia. The simulated surface PM2.5 chemical components via the two modules showed the largest systematic biases in surface OC, with a mean bias of 4.5 μg m−3, and the second largest in SO42− abundance of 2.2 μg m−3 over Seoul. Compared with surface observations at two ground sites located near the western coastal Korean Peninsula, MADE/VBS exhibited the overpredictions in OC by 170–180%, whereas MADE/SORGAM showed underpredictions by 49–65%. OC and sulfate via MADE/VBS were simulated to be much higher than that simulated by MADE/SORGAM by a factor of 2.8–3.5 and 1.5–1.9, respectively. Model verification against KORUS-AQ aircraft measurements also showed large discrepancies in simulated non-surface OC between the two modules by a factor of five, with higher OC by MADE/VBS and lower IC by MADE/SORGAM, whereas much closer MADE/VBS simulations to the KORUS-AQ aircraft measurements were found. On the basis of the aircraft measurements, the aggregated bias (sum of four components) for PM2.5 mass concentrations from the MADE/VBS module indicated that the simulation was much closer to the measurements, nevertheless more elaborate analysis on the surface OC simulation performance would be needed to improve the ground results. Our findings show that significant inconsistencies are present in the secondary organic aerosol formation simulations, suggesting that PM2.5 forecasts should be considered with great caution, as well as in the context of policymaking in the Northeast Asia region.


2021 ◽  
Author(s):  
Matthias Karl ◽  
Liisa Pirjola ◽  
Tiia Grönholm ◽  
Mona Kurppa ◽  
Srinivasan Anand ◽  
...  

Abstract. Numerical models are needed for evaluating aerosol processes in the atmosphere in state-of-the-art chemical transport models, urban-scale dispersion models and climatic models. This article describes a publicly available aerosol dynamics model MAFOR (Multicomponent Aerosol FORmation model; version 2.0); we address the main structure of the model, including the types of operation and the treatments of the aerosol processes. The main advantage of MAFOR v2.0 is the consistent treatment of both the mass- and number-based concentrations of particulate matter. An evaluation of the model is also presented, against a high-resolution observational dataset in a street canyon located in the centre of Helsinki (Finland) during an afternoon traffic rush hour on 13 December 2010. The experimental data included measurements at different locations in the street canyon of ultrafine particles, black carbon, and fine particulate mass PM1. This evaluation has also included an intercomparison with the corresponding predictions of two other prominent aerosol dynamics models, AEROFOR and SALSA. All three models fairly well simulated the decrease of the measured total particle number concentrations with increasing distance from the vehicular emission source. The MAFOR model reproduced the evolution of the observed particle number size distributions more accurately than the other two models. The MAFOR model also predicted the variation of the concentration of PM1 better than the SALSA model. We also analysed the relative importance of various aerosol processes based on the predictions of the three models. As expected, atmospheric dilution dominated over other processes; dry deposition was the second most significant process. Numerical sensitivity tests with the MAFOR model revealed that the uncertainties associated with the properties of the condensing organic vapours affected only the size range of particles smaller than 10 nm in diameter. These uncertainties do not therefore affect significantly the predictions of the whole of the number size distribution and the total number concentration. The MAFOR model version 2 is well documented and versatile to use, providing a range of alternative parametrizations for various aerosol processes. The model includes an efficient numerical integration of particle number and mass concentrations, an operator-splitting of processes, and the use of a fixed sectional method. The model could be used as a module in various atmospheric and climatic models.


2011 ◽  
Vol 11 (12) ◽  
pp. 5897-5915 ◽  
Author(s):  
P. Roldin ◽  
E. Swietlicki ◽  
A. Massling ◽  
A. Kristensson ◽  
J. Löndahl ◽  
...  

Abstract. The climate effects downwind of an urban area resulting from gaseous and particulate emissions within the city are as yet inadequately quantified. The aim of this work was to estimate these effects for Malmö city in southern Sweden (population 280 000). The chemical and physical particle properties were simulated with a model for Aerosol Dynamics, gas phase CHEMistry and radiative transfer calculations (ADCHEM) following the trajectory movement from upwind of Malmö, through the urban background environment and finally tens and hundreds of kilometers downwind of Malmö. The model results were evaluated using measurements of the particle number size distribution and chemical composition. The total particle number concentration 50 km (~ 3 h) downwind, in the center of the Malmö plume, is about 3700 cm−3 of which the Malmö contribution is roughly 30%. Condensation of nitric acid, ammonium and to a smaller extent oxidized organic compounds formed from the emissions in Malmö increases the secondary aerosol formation with a maximum of 0.7–0.8 μg m−3 6 to 18 h downwind of Malmö. The secondary mass contribution dominates over the primary soot contribution from Malmö already 3 to 4 h downwind of the emission sources and contributes to an enhanced total surface direct or indirect aerosol shortwave radiative forcing in the center of the urban plume ranging from −0.3 to −3.3 W m−2 depending on the distance from Malmö, and the specific cloud properties.


1998 ◽  
Vol 32 (17) ◽  
pp. 2981-2999 ◽  
Author(s):  
Ingmar J. Ackermann ◽  
Heinz Hass ◽  
M. Memmesheimer ◽  
A. Ebel ◽  
Francis S. Binkowski ◽  
...  

2010 ◽  
Vol 10 (8) ◽  
pp. 18731-18780 ◽  
Author(s):  
P. Roldin ◽  
E. Swietlicki ◽  
A. Massling ◽  
A. Kristensson ◽  
J. Löndahl ◽  
...  

Abstract. The climate and health effects downwind of an urban area resulting from gaseous and particulate emissions within the city are as yet inadequately quantified. The aim of this work was to estimate these effects for Malmö city in Southern Sweden (population 280 000). The chemical and physical particle properties were simulated with a model for Aerosol Dynamics, gas phase CHEMistry and radiative transfer calculations (ADCHEM) following the trajectory movement from upwind Malmö, through the urban background environment and finally tens and hundreds of kilometers downwind Malmö. The model results were validated with measurements of the particle number size distribution and chemical composition. The total particle number concentration 50 km (~3 h) downwind in the center of the Malmö plume is about 3800 cm−3 and the Malmö contribution is roughly 35%. Condensation of nitric acid, ammonium and to a smaller extent oxidized organic compounds formed from the emissions in Malmö increases the secondary aerosol formation with a maximum of 0.6–0.7 μg/m3 6 to 18 h downwind of Malmö. The secondary mass contribution dominates over the primary soot contribution from Malmö already 2 to 3 h after the emissions and gives an enhanced total top of the atmosphere direct or indirect aerosol shortwave radiative forcing in the center of the urban plume ranging from −0.3 to −2.3 W m−2 depending on the distance from Malmö, and the cloud properties. It also gives an increased respiratory tract deposited mass dose, which increases with the distance downwind Malmö.


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