Aerosol microphysical processes are essential for the next generation of global and regional climate and air quality models to determine particle size distribution. The contribution of organic aerosols (OAs) to particle formation, mass, and number concentration is one of the major uncertainties in current models. A new global–regional nested aerosol model was developed to simulate detailed microphysical processes. The model combines an advanced particle microphysics (APM) module and a volatility basis set (VBS) OA module to calculate the kinetic condensation of low-volatility organic compounds and equilibrium partitioning of semi-volatile organic compounds in a 3-D framework using global–regional nested domain. In addition to the condensation of sulfuric acid, the equilibrium partitioning of nitrate and ammonium, and the coagulation process of particles, the microphysical processes of the OAs are realistically represented in our new model. The model uses high-resolution size bins to calculate the size distribution of new particles formed through nucleation and subsequent growth. The multi-scale nesting enables the model to perform high-resolution simulations of the particle formation processes in the urban atmosphere in the background of regional and global environments. By using the nested domains, the model reasonably reproduced the OA components obtained from the analysis of aerosol mass spectrometry measurements through positive matrix factorization and the particle number size distribution in the megacity of Beijing during a period of approximately a month. Anthropogenic organic species accounted for 67 % of the OAs of secondary particles formed by nucleation and subsequent growth, which is considerably larger than that of biogenic OAs. On the global scale, the model well predicted the particle number concentration in various environments. The microphysical module combined with the VBS simulated the universal distribution of organic components among the different aerosol populations. The model results strongly suggest the importance of anthropogenic organic species in aerosol particle formation and growth at polluted urban sites and over the whole globe.
Dust aerosol has important climate and environmental effects, which could be changed by internally mixing with anthropogenic aerosol as a result of heterogeneous reactions; however, the importance of these reactions is not fully understood yet. In this study, synergetic observations and an air quality model were used to analyze the transport of a severe dust storm and its impacts on nitrate and sulfate levels over East Asia between 3 and 11 May 2017. The model successfully reproduced the occurrence and transport of the dust storm compared to dust RGB imageries of the Himawari-8 satellite and dust extinction coefficients observed by LIDAR. The model also reasonably simulated the variations of observed nitrate and sulfate concentrations, and the results indicated that the dust heterogeneous reactions were dominant pathways for nitrate formation, but they had limited contribution for sulfate in both fine and coarse mode in Fukuoka, Japan. Dust nitrate formed rapidly after leaving China, and the highest period-averaged concentration of dust nitrate (>5 μg m−3) was shown over the Yellow Sea. Based on model results; we found that the mass ratio of dust nitrate to dust aerosol could reach 10% over the Pacific Ocean. Our results confirmed the importance of heterogeneous reactions on compositions of dust particles.
18 December 2024 in Geoscientific Model Development
Polycyclic aromatic hydrocarbons (PAHs) significantly impact human health due to their persistence, toxicity, and potential carcinogenicity. Their global distribution and regional changes caused by emission changes, especially over areas in developing countries, remain to be understood along with their health impacts. This study implemented a PAH module in the global–regional nested Atmospheric Aerosol and Chemistry Model of the Institute of Atmospheric Physics (IAP-AACM) to investigate the global distribution of PAHs and the change in their health risks from 2013 to 2018 in China. An evaluation against observations showed that the model could capture well the spatial distribution and seasonal variation in Benzo[a]pyrene (BaP), the typical indicator species of PAHs. On a global scale, the annual mean concentrations are the highest in China followed by Europe and India, with high values exceeding the target values of 1 ng m−3 over some areas. Compared with 2013, the concentration of BaP in China decreased in 2018 due to emission reductions, whereas it increased in India and southern Africa. However, the decline is much smaller than for PM2.5 during the same period. The concentration of BaP decreased by 8.5 % in Beijing–Tianjin–Hebei (BTH) and 9.4 % in the Yangtze River Delta (YRD). It even increased over areas in the Sichuan Basin due to changes in meteorological conditions. The total incremental lifetime cancer risk (ILCR) posed by BaP only showed a slight decrease in 2018, and the population in east China still faced significant potential health risks. The results indicate that strict additional control measures should be taken to reduce the pollution and health risks of PAHs effectively. The study also highlights the importance of considering changes in meteorological conditions when evaluating emission changes from concentration monitoring.
Atmospheric ammonia (NH3) plays an important role in the formation of secondary inorganic aerosols, the neutralization of acid rain, and the deposition to ecosystems, but has not been well understood yet, especially over East Asia. Based on the GEOS-Chem model results, the IASI satellite retrievals, the in-site surface observations of a nationwide filter pack (FP) network over Japan and the long-term high resolution online NH3 measurements at Fukuoka of western Japan, the spatio-temporal distributions of atmospheric NH3 over East Asia was analyzed comprehensively. A significant seasonal variation with a summer peak was found in all datasets. Comparison between the satellite retrievals and model simulations indicated that the IASI NH3 vertical column density (VCD) showed good consistency with GEOS-Chem results over North and central China, but had large differences over South China due to the effect of clouds. Over the Japan area, GEOS-Chem simulated NH3 concentrations successfully reproduced the spatio-temporal variations compared with in-situ observations, while IASI NH3 VCD retrievals were below or near the detection limit and difficult to obtain a reasonable correlation for with model results. The comprehensive analysis indicated that there were still some differences among different datasets, and more in-situ observations, improved satellite retrievals, and high-resolution model simulations with more accurate emissions are necessary for better understanding the atmospheric NH3 over East Asia.