scholarly journals Improvement of inorganic aerosol component in PM<sub>2.5</sub> by constraining aqueous-phase formation of sulfate in cloud with satellite retrievals: WRF-Chem simulations

2020 ◽  
Author(s):  
Tong Sha ◽  
Xiaoyan Ma ◽  
Jun Wang ◽  
Rong Tian ◽  
Jianqi Zhao ◽  
...  

Abstract. High concentrations of PM2.5 in China have caused severe visibility degradation and health problem. However, it is still a big challenge to accurately predict PM2.5 and its chemical components in the numerical model. In this study, we compared the inorganic aerosol components of PM2.5 (sulfate, nitrate, and ammonium (SNA)) simulated by WRF-Chem with in-situ data during a heavy haze-fog event (November 2018) in Nanjing. The comparisons show that the model underestimates the sulfate concentrations by 81 % and fails to reproduce the significant increase of sulfate concentrations from early morning to noon, which corresponds to the timing of fog dissipation, suggesting that the model underestimates the aqueous-phase formation of sulfate in clouds. In addition, the model overestimates both nitrate and ammonium concentrations by 184 % and 57 %, respectively. These ultimately result in the simulated SNA 77.2 % higher than the observations. However, as the important aqueous-phase reactors, cloud water are simultaneously underestimated by the model. Therefore, the modeled cloud water was constrained based on the MODIS Liquid Water Path (LWP) observations. Results show that the simulation with MODIS-corrected cloud water amount increases the sulfate by a factor of 3, decreases NMB by 53.5 %, and can reproduce its diurnal cycles, i.e. the peak concentration at noon. Also, the model absolute bias of nitrate decreases from 184 % to 50 %, especially for the nocturnal concentrations, which suggests the MODIS-constrained simulation improved the diurnal pattern. Although the simulated ammonium is still higher than the observation, corrected cloud water lead to the decrease of the modeled bias of SNA from 77.2 % to 14.1 %. The strong sensitivity of simulated SNA concentration to the cloud water provides an explanation for the bias of SNA simulation. Hence, the uncertainties of cloud water can lead to model bias in simulating SNA, and can be reduced by constraining the model with satellite observations.

2009 ◽  
Vol 137 (3) ◽  
pp. 1083-1110 ◽  
Author(s):  
Andrew S. Ackerman ◽  
Margreet C. vanZanten ◽  
Bjorn Stevens ◽  
Verica Savic-Jovcic ◽  
Christopher S. Bretherton ◽  
...  

Abstract Cloud water sedimentation and drizzle in a stratocumulus-topped boundary layer are the focus of an intercomparison of large-eddy simulations. The context is an idealized case study of nocturnal stratocumulus under a dry inversion, with embedded pockets of heavily drizzling open cellular convection. Results from 11 groups are used. Two models resolve the size distributions of cloud particles, and the others parameterize cloud water sedimentation and drizzle. For the ensemble of simulations with drizzle and cloud water sedimentation, the mean liquid water path (LWP) is remarkably steady and consistent with the measurements, the mean entrainment rate is at the low end of the measured range, and the ensemble-average maximum vertical wind variance is roughly half that measured. On average, precipitation at the surface and at cloud base is smaller, and the rate of precipitation evaporation greater, than measured. Including drizzle in the simulations reduces convective intensity, increases boundary layer stratification, and decreases LWP for nearly all models. Including cloud water sedimentation substantially decreases entrainment, decreases convective intensity, and increases LWP for most models. In nearly all cases, LWP responds more strongly to cloud water sedimentation than to drizzle. The omission of cloud water sedimentation in simulations is strongly discouraged, regardless of whether or not precipitation is present below cloud base.


2022 ◽  
pp. 1-48
Author(s):  
Yi Ming

Abstract A negative shortwave cloud feedback associated with higher extratropical liquid water content in mixed-phase clouds is a common feature of global warming simulations, and multiple mechanisms have been hypothesized. A set of process-level experiments performed with an idealized global climate model (a dynamical core with passive water and cloud tracers and full Rotstayn-Klein single-moment microphysics) show that the common picture of the liquid water path (LWP) feedback in mixed-phase clouds being controlled by the amount of ice susceptible to phase change is not robust. Dynamic condensate processes—rather than static phase partitioning—directly change with warming, with varied impacts on liquid and ice amounts. Here, three principal mechanisms are responsible for the LWP response, namely higher adiabatic cloud water content, weaker liquid-to-ice conversion through the Bergeron-Findeisen process, and faster melting of ice and snow to rain. Only melting is accompanied by a substantial loss of ice, while the adiabatic cloud water content increase gives rise to a net increase in ice water path (IWP) such that total cloud water also increases without an accompanying decrease in precipitation efficiency. Perturbed parameter experiments with a wide range of climatological LWP and IWP demonstrate a strong dependence of the LWP feedback on the climatological LWP and independence from the climatological IWP and supercooled liquid fraction. This idealized setup allows for a clean isolation of mechanisms and paints a more nuanced picture of the extratropical mixed-phase cloud water feedback than simple phase change.


2016 ◽  
Author(s):  
Weihua Chen ◽  
Xuemei Wang ◽  
Jason Blake Cohen ◽  
Shengzhen Zhou ◽  
Zhisheng Zhang ◽  
...  

Abstract. Measurements of size-resolved aerosols from 0.25 to 18 μm were conducted at three sites (urban, suburban and background sites) and used in tandem with an atmospheric transport model to study the size distribution and formation of atmospheric aerosols in southern China during the monsoon season (May–June) in 2010. The mass distribution showed the majority of chemical components were found in the smaller size bins (< 2.5 μm). Sulfate, was found to be strongly correlated with aerosol water, and anti-correlated with atmospheric SO2, hinting at aqueous-phase reactions being the main formation pathway. Nitrate was the only major species that showed a bi-modal distribution at the urban site, and was dominated by the coarse mode in the other two sites, suggesting that an important component of nitrate formation is chloride depletion of sea salt transported from the South China Sea. In addition to these aqueous-phase reactions and interactions with sea salt aerosols, new particle formation, chemical aging, and long-range transport from upwind urban or biomass burning regions were also found to be important in at least some of the sights on some of the days. This work therefore summarizes the different mechanisms that significantly impact the aerosol chemical composition during the Monsoon over southern China.


2016 ◽  
Vol 16 (11) ◽  
pp. 7357-7371 ◽  
Author(s):  
Mi Tian ◽  
Huanbo Wang ◽  
Yang Chen ◽  
Fumo Yang ◽  
Xiaohua Zhang ◽  
...  

Abstract. Extremely severe haze weather events occurred in many cities in China, especially in the east part of the country, in January 2013. Comprehensive measurements including hourly concentrations of PM2.5 and its major chemical components (water-soluble inorganic ions, organic carbon (OC), and elemental carbon (EC)) and related gas-phase precursors were conducted via an online monitoring system in Suzhou, a medium-sized city in Jiangsu province, just east of Shanghai. PM2.5 (particulate matter with an aerodynamic diameter of 2.5 µm or less) frequently exceeded 150 µg m−3 on hazy days, with the maximum reaching 324 µg m−3 on 14 January 2013. Unfavorable weather conditions (high relative humidity (RH), and low rainfall, wind speed, and atmospheric pressure) were conducive to haze formation. High concentrations of secondary aerosol species (including SO42−, NO3−, NH4+, and SOC) and gaseous precursors were observed during the first two haze events, while elevated primary carbonaceous species emissions were found during the third haze period, pointing to different haze formation mechanisms. Organic matter (OM), (NH4)2SO4, and NH4NO3 were found to be the major contributors to visibility impairment. High concentrations of sulfate and nitrate might be explained by homogeneous gas-phase reactions under low RH conditions and by heterogeneous processes under relatively high RH conditions. Analysis of air mass trajectory clustering and potential source contribution function showed that aerosol pollution in the studied areas was mainly caused by local activities and surrounding sources transported from nearby cities.


2013 ◽  
Vol 70 (8) ◽  
pp. 2393-2408 ◽  
Author(s):  
David Painemal ◽  
Patrick Minnis ◽  
Larry O'Neill

Abstract The diurnal cycles in cloud-top height Htop and cloud fraction (CF) in the southeastern Pacific stratocumulus region were determined for October–November 2008 by analyzing data from Geostationary Operational Environmental Satellite-10 (GOES-10) according to a diurnal/semidiurnal harmonic fitting technique. The value of Htop was obtained by applying a formula based on a linear regression of the differences between GOES-10 cloud-top temperature and Tropical Rainfall Measuring Mission (TRMM) Microwave Imager (TMI) satellite sea surface temperature, with a common 0.25° × 0.25° spatial resolution. A satellite liquid water path (LWP) climatology complemented this dataset. Southwestward transects of Htop and LWP anomalies reveal a coherent propagating signal from the coast in the afternoon, with a typical phase speed of 25 m s−1. This pattern is preceded by a subsidence wave that reaches its peak a few hours before the maximum in Htop and LWP anomalies. Coincident increases in LWP and Htop after the subsidence wave passes suggest that the boundary layer deepening promotes cloud thickening and increased LWP, which are likely maintained through a well-mixed boundary layer and sufficient moisture fluxes that can counteract the effect of dry air entrainment. The interference between the radiatively and subsidence wave–driven cycles gives rise to a semidiurnal cycle in Htop along the coast. While the semidiurnal amplitude is near 80 m close to the coast with a fraction of explained variance greater than 0.4, it decreases to 30 m offshore (80°W). Similar to Htop, CF also exhibits contrasting zonal differences, but with a smaller semidiurnal component. The phase of the semidiurnal harmonic resembles the subsidence propagation westward, and the noticeable land–sea breeze circulation at 26°S that extends 200 km offshore.


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