skip to main content


Title: Chemical Data Assimilation With Aqueous Chemistry in WRF‐Chem Coupled With WRFDA (V4.4.1)
Abstract

This study introduces a new chemistry option in the Weather Research and Forecasting model data assimilation (WRFDA) system, coupled with the WRF‐Chem model (Version 4.4.1), to incorporate aqueous chemistry (AQCHEM) in the assimilation of ground‐level chemical measurements. The new DA capability includes the integration of aqueous‐phase aerosols from the Regional Atmospheric Chemistry Mechanism (RACM) gas chemistry, the Modal Aerosol Dynamics Model for Europe (MADE) aerosol chemistry, and the Volatility Basis Set (VBS) for secondary organic aerosol production. The RACM‐MADE‐VBS‐AQCHEM scheme facilitates aerosol‐cloud‐precipitation interactions by activating aerosol particles in cloud water during the model simulation. With the goal of enhancing air quality forecasting in cloudy conditions, this new implementation is demonstrated in the weakly coupled three‐dimensional variational data assimilation (3D‐Var) system through regional air quality cycling over East Asia. Surface particulate matter (PM) concentrations and four gas species (SO2, NO2, O3, and CO) are assimilated every 6 hr for the month of March 2019. The results show that including aqueous‐phase aerosols in both the analysis and forecast can represent aerosol wet removal processes associated with cloud development and rainfall production. During a pollution event with high cloud cover, simulations without aerosols defined in cloud water exhibit significantly higher values for liquid water path, and surface PM10(PM2.5) concentrations are overestimated by a factor of 10 (3) when wet scavenging processes dominate. On the contrary, AQCHEM proves to be helpful in simulating the wet deposition of aerosols, accurately predicting the evolution of surface PM concentrations without such overestimation.

 
more » « less
NSF-PAR ID:
10492305
Author(s) / Creator(s):
 ;  ;  ;  ;  ;  ;  
Publisher / Repository:
DOI PREFIX: 10.1029
Date Published:
Journal Name:
Journal of Advances in Modeling Earth Systems
Volume:
16
Issue:
2
ISSN:
1942-2466
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. Abstract

    Deep convection can transport surface moisture and pollution from the planetary boundary layer to the upper troposphere (UT) within a few minutes. The convective transport of precursors of both ozone and aerosols from the planetary boundary layer affects the concentrations of these constituents in the UT and can influence the Earth's radiation budget and climate. Some precursors of both ozone and aerosols are soluble and reactive in the aqueous phase. This study uses the Weather Research and Forecasting model coupled with Chemistry (WRF‐Chem) to simulate the wet scavenging of precursors of both ozone and aerosols including CH2O, CH3OOH, H2O2, and SO2in a supercell system observed on 29 May 2012, during the 2012 Deep Convective Clouds and Chemistry (DC3) field campaign at cloud‐parameterized resolution. The default WRF‐Chem simulations underestimate the mixing ratios of soluble ozone precursors in the UT because the dissolved soluble trace gases are not released when the droplets freeze. In order to improve the model simulation of cloud‐parameterized wet scavenging, we added ice retention factors for various species to the cloud‐parameterized wet scavenging module and adjusted the conversion rate of cloud water to rainwater at temperatures below freezing in the cloud parameterization as well as in the subgrid‐scale wet‐scavenging calculation. The introduction of these model modifications greatly improved the model simulation of less soluble species.

     
    more » « less
  2. Abstract

    Since 2013, Chinese policies have dramatically reduced emissions of particulates and their gas‐phase precursors, but the implications of these reductions for aerosol‐radiation interactions are unknown. Using a global, coupled chemistry‐climate model, we examine how the radiative impacts of Chinese air pollution in the winter months of 2012 and 2013 affect local meteorology and how these changes may, in turn, influence surface concentrations of PM2.5, particulate matter with diameter <2.5 μm. We then investigate how decreasing emissions through 2016 and 2017 alter this impact. We find that absorbing aerosols aloft in winter 2012 and 2013 heat the middle‐ and lower troposphere by ∼0.5–1 K, reducing cloud liquid water, snowfall, and snow cover. The subsequent decline in surface albedo appears to counteract the ∼15–20 W m−2decrease in shortwave radiation reaching the surface due to attenuation by aerosols overhead. The net result of this novel cloud‐snowfall‐albedo feedback in winters 2012–2013 is a slight increase in surface temperature of ∼0.5–1 K in some regions and little change elsewhere. The aerosol heating aloft, however, stabilizes the atmosphere and decreases the seasonal mean planetary boundary layer (PBL) height by ∼50 m. In winter 2016 and 2017, the ∼20% decrease in mean PM2.5weakens the cloud‐snowfall‐albedo feedback, though it is still evident in western China, where the feedback again warms the surface by ∼0.5–1 K. Regardless of emissions, we find that aerosol‐radiation interactions enhance mean surface PM2.5pollution by 10%–20% across much of China during all four winters examined, mainly though suppression of PBL heights.

     
    more » « less
  3. Abstract

    This paper examines the accuracy of Weather Research and Forecasting model coupled with Chemistry (WRF‐Chem) generated 72 hr fine particulate matter (PM2.5) forecasts in Delhi during the crop residue burning season of October‐November 2017 with respect to assimilation of the Moderate Resolution Imaging Spectroradiometer (MODIS) aerosol optical depth (AOD) retrievals, persistent fire emission assumption, and aerosol‐radiation interactions. The assimilation significantly pushes the model AOD and PM2.5toward the observations with the largest changes below 5 km altitude in the fire source regions (northeastern Pakistan, Punjab, and Haryana) as well as the receptor New Delhi. WRF‐Chem forecast with MODIS AOD assimilation, aerosol‐radiation feedback turned on, and real‐time fire emissions reduce the mean bias by 88–195 μg/m3(70–86%) with the largest improvement during the peak air pollution episode of 6–13 November 2017. Aerosol‐radiation feedback contributes ~21%, ~25%, and ~24% to reduction in mean bias of the first, second, and third days of PM2.5forecast. Persistence fire emission assumption is found to work really well, as the accuracy of PM2.5forecasts driven by persistent fire emissions was only 6% lower compared to those driven by real fire emissions. Aerosol‐radiation feedback extends the benefits of assimilating satellite AOD beyond PM2.5forecasts to surface temperature forecast with a reduction in the mean bias of 0.9–1.5°C (17–30%). These results demonstrate that air quality forecasting can benefit substantially from satellite AOD observations particularly in developing countries that lack resources to rapidly build dense air quality monitoring networks.

     
    more » « less
  4. Abstract. Marine emissions of dimethyl sulfide (DMS) and the subsequent formation of its oxidation products methanesulfonic acid (MSA) and sulfuric acid (H2SO4) are well-known natural precursors of atmospheric aerosols, contributing to particle mass and cloud formation over ocean and coastal regions. Despite a long-recognized and well-studied role in the marine troposphere, DMS oxidation chemistry remains a work in progress within many current air quality and climate models, with recent advances exploring heterogeneous chemistry and uncovering previously unknown intermediate species. With the identification of additional DMS oxidation pathways and intermediate species that influence the eventual fate of DMS, it is important to understand the impact of these pathways on the overall sulfate aerosol budget and aerosol size distribution. In this work, we update and evaluate the DMS oxidation mechanism of the chemical transport model GEOS-Chem by implementing expanded DMS oxidation pathways in the model. These updates include gas- and aqueous-phase reactions, the formation of the intermediates dimethyl sulfoxide (DMSO) and methanesulfinic acid (MSIA), and cloud loss and aerosol uptake of the recently quantified intermediate hydroperoxymethyl thioformate (HPMTF). We find that this updated mechanism collectively decreases the global mean surface-layer gas-phase sulfur dioxide (SO2) mixing ratio by 40 % and enhances the sulfate aerosol (SO42-) mixing ratio by 17 %. We further perform sensitivity analyses exploring the contribution of cloud loss and aerosol uptake of HPMTF to the overall sulfur budget. Comparing modeled concentrations to available observations, we find improved biases relative to previous studies. To quantify the impacts of these chemistry updates on global particle size distributions and the mass concentration, we use the TwO-Moment Aerosol Sectional (TOMAS) aerosol microphysics module coupled to GEOS-Chem and find that changes in particle formation and growth affect the size distribution of aerosol. With this new DMS-oxidation scheme, the global annual mean surface-layer number concentration of particles with diameters smaller than 80 nm decreases by 16.8 %, with cloud loss processes related to HPMTF being mostly responsible for this reduction. However, the global annual mean number of particles larger than 80 nm (corresponding to particles capable of acting as cloud condensation nuclei, CCN) increases by 3.8 %, suggesting that the new scheme promotes seasonal particle growth to these sizes.

     
    more » « less
  5. Abstract. Heterogeneous chemistry of oxidized carbons in aerosol phase is known to significantly contribute to secondary organic aerosol (SOA) burdens. TheUNIfied Partitioning Aerosol phase Reaction (UNIPAR) model was developed to process the multiphase chemistry of various oxygenated organics into SOAmass predictions in the presence of salted aqueous phase. In this study, the UNIPAR model simulated the SOA formation from gasoline fuel, which is amajor contributor to the observed concentration of SOA in urban areas. The oxygenated products, predicted by the explicit mechanism, were lumpedaccording to their volatility and reactivity and linked to stoichiometric coefficients which were dynamically constructed by predetermined mathematical equations at different NOx levels and degrees of gas aging. To improve the model feasibility in regional scales, the UNIPAR model was coupled with the Carbon Bond 6 (CB6r3) mechanism. CB6r3 estimated the hydrocarbon consumption and the concentration of radicals (i.e., RO2 and HO2) to process atmospheric aging of gas products. The organic species concentrations, estimated bystoichiometric coefficient array and the consumption of hydrocarbons, were applied to form gasoline SOA via multiphase partitioning andaerosol-phase reactions. To improve the gasoline SOA potential in ambient air, model parameters were also corrected for gas–wall partitioning(GWP). The simulated gasoline SOA mass was evaluated against observed data obtained in the University of Florida Atmospheric PHotochemical Outdoor Reactor (UF-APHOR) chamber under varying sunlight, NOx levels, aerosol acidity, humidity, temperature, and concentrations of aqueous salts and gasoline vapor. Overall, gasoline SOAwas dominantly produced via aerosol-phase reaction, regardless of the seed conditions owing to heterogeneous reactions of reactive multifunctionalorganic products. Both the measured and simulated gasoline SOA was sensitive to seed conditions showing a significant increase in SOA mass with increasing aerosol acidity and water content. A considerable difference in SOA mass appeared between two inorganic aerosol states (dry aerosol vs. wet aerosol) suggesting a large difference in SOA formation potential between arid (western United States) and humid regions (eastern United States). Additionally, aqueous reactions of organic products increased the sensitivity of gasoline SOA formation to NOx levels as well as temperature. The impact of the chamber wall on SOA formation was generally significant, and it appeared to be higher in the absence of wet salts. Based on the evaluation of UNIPAR against chamber data from 10 aromatic hydrocarbons and gasoline fuel, we conclude that the UNIPAR model with both heterogeneous reactions and the model parameters corrected for GWP can improve the ability to accurately estimate SOA mass in regional scales. 
    more » « less