Analysis of atmospheric ammonia over South and East Asia based on the MOZART-4 model and its comparison with satellite and surface observations

Limited availability of atmospheric ammonia (NH3) observations limits our understanding of controls on its spatial and temporal variability and its interactions with the ecosystem. Here we used the Model for Ozone and Related chemical Tracers version 4 (MOZART-4) global chemistry transport model and the Hemispheric Transport of Air Pollution version 2 (HTAP-v2) emission inventory to simulate global NH3 distribution for the year 2010. We presented a first comparison of the model with monthly averaged satellite distributions and limited ground-based observations available across South Asia. The MOZART-4 simulations over South Asia and East Asia were evaluated with the NH3 retrievals obtained from the Infrared Atmospheric Sounding Interferometer (IASI) satellite and 69 ground-based monitoring stations for air quality across South Asia and 32 ground-based monitoring stations from the Nationwide Nitrogen Deposition Monitoring Network (NNDMN) of China. We identified the northern region of India (Indo-Gangetic Plain, IGP) as a hotspot for NH3 in Asia, both using the model and satellite observations. In general, a close agreement was found between yearly averaged NH3 total columns simulated by the model and IASI satellite measurements over the IGP, South Asia (r=0.81), and the North China Plain (NCP), East Asia (r=0.90). However, the MOZART-4-simulated NH3 column was substantially higher over South Asia than East Asia, as compared with the IASI retrievals, which show smaller differences. Model-simulated surface NH3 concentrations indicated smaller concentrations in all seasons than surface NH3 measured by the ground-based observations over South and East Asia, although uncertainties remain in the available surface NH3 measurements. Overall, the comparison of East Asia and South Asia using both MOZART-4 model and satellite observations showed smaller NH3 columns in East Asia compared with South Asia for comparable emissions, indicating rapid dissipation of NH3 due to secondary aerosol formation, which can be explained by larger emissions of acidic precursor gases in East Asia

Performance of WRF-Chem over Indian region: Comparison with measurements

The aerosol mass concentrations over several Indian regions have been simulated using the online chemistry transport model, WRF-Chem, for two distinct seasons of 2011, representing the pre-monsoon (May) and post-monsoon (October) periods during the Indo-US joint experiment `Ganges Valley Aerosol Experiment (GVAX)'. The simulated values were compared with concurrent measurements. It is found that the model systematically underestimates near-surface BC mass concentrations as well as columnar Aerosol Optical Depths (AODs) from the measurements. Examining this in the light of the model-simulated meteorological parameters, we notice the model overestimates both planetary boundary layer height (PBLH) and surface wind speeds, leading to deeper mixing and dispersion and hence lower surface concentrations of aerosols. Shortcoming in simulating rainfall pattern also has an impact through the scavenging effect. It also appears that the columnar AODs are influenced by the unrealistic emission scenarios in the model. Comparison with vertical profiles of BC obtained from aircraft-based measurements also shows a systematic underestimation by the model at all levels. It is seen that concentration of other aerosols, viz., dust and sea-salt are closely linked with meteorological conditions prevailing over the region. Dust is higher during pre-monsoon periods due to the prevalence of north-westerly winds that advect dust from deserts of west Asia into the Indo-Gangetic plain. Winds and rainfall influence sea-salt concentrations. Thus, the unrealistic simulation of wind and rainfall leads to model simulated dust and sea-salt also to deviate from the real values; which together with BC also causes underperformance of the model with regard to columnar AOD. It appears that for better simulations of aerosols over Indian region, the model needs an improvement in the simulation of the meteorology

Simulations of black carbon over the Indian region: improvements and implications of diurnality in emissions

With a view to improving the performance of WRF-Chem over the Indian region in simulating BC (black carbon) mass concentrations as well as its short-term variations, especially on a diurnal scale, a region-specific diurnal variation scheme has been introduced in the model emissions and the performance of the modified simulations has been evaluated against high-resolution measurements carried out over eight ARFI (Aerosol Radiative Forcing over India) network observatories spread across India for distinct seasons: pre-monsoon (represented by May), post-monsoon (represented by October) and winter (represented by December). In addition to an overall improvement in the simulated concentrations and their temporal variations, we have also found that the effects of prescribing diurnally varying emissions on the simulated near-surface concentrations largely depend on the boundary layer turbulence. The effects are perceived quickly (within about 2-3 h) during the evening-early morning hours when the atmospheric boundary layer is shallow and convective mixing is weak, while they are delayed, taking as much as about 5-6 h, during periods when the boundary layer is deep and convective mixing is strong. This information would also serve as an important input for agencies concerned with urban planning and pollution mitigation. Despite these improvements in the near-surface concentrations, the simulated columnar aerosol optical depth (AOD) still remains largely underestimated vis-a-vis the satellite-retrieved products. These modifications will serve as a guideline for further model-improvement initiatives at a regional scale

Inter-comparison and performance evaluation of chemistry transport models over Indian region

Aerosol loading over the South Asian region has the potential to affect the monsoon rainfall, Himalayan glaciers and regional air-quality, with implications for the billions in this region. While field campaigns and network observations provide primary data, they tend to be location/season specific. Numerical models are useful to regionalize such location-specific data. Studies have shown that numerical models underestimate the aerosol scenario over the Indian region, mainly due to shortcomings related to meteorology and the emission inventories used. In this context, we have evaluated the performance of two such chemistry-transport models: WRF-Chem and SPRINTARS over an India-centric domain. The models differ in many aspects including physical domain, horizontal resolution, meteorological forcing and so on etc. Despite these differences, both the models simulated similar spatial patterns of Black Carbon (BC) mass concentration, (with a spatial correlation of 0.9 with each other), and a reasonable estimates of its concentration, though both of them under-estimated vis-a-vis the observations. While the emissions are lower (higher) in SPRINTARS (WRF-Chem), overestimation of wind parameters in WRF-Chem caused the concentration to be similar in both models. Additionally, we quantified the under-estimations of anthropogenic BC emissions in the inventories used these two models and three other widely used emission inventories. Our analysis indicates that all these emission inventories underestimate the emissions of BC over India by a factor that ranges from 1.5 to 2.9. We have also studied the model simulations of aerosol optical depth over the Indian region. The models differ significantly in simulations of AOD, with WRF-Chem having a better agreement with satellite observations of AOD as far as the spatial pattern is concerned. It is important to note that in addition to BC, dust can also contribute significantly to AOD. The models differ in simulations of the spatial pattern of mineral dust over the Indian region. We find that both meteorological forcing and emission formulation contribute to these differences. Since AOD is column integrated parameter, description of vertical profiles in both models, especially since elevated aerosol layers are often observed over Indian region, could be also a contributing factor. Additionally, differences in the prescription of the optical properties of BC between the models appear to affect the AOD simulations. We also compared simulation of sea-salt concentration in the two models and found that WRF-Chem underestimated its concentration vis-a-vis SPRINTARS. The differences in near-surface oceanic wind speeds appear to be the main source of this difference. In-spite of these differences, we note that there are similarities in their simulation of spatial patterns of various aerosol species (with each other and with observations) and hence models could be valuable tools for aerosol-related studies over the Indian region. Better estimation of emission inventories could improve aerosol-related simulations. (C) 2015 Elsevier Ltd. All rights reserved

Black carbon emissions and its impact on the monsoon rainfall patterns over the Indian subcontinent: Insights into localized warming effects

This study investigates the impact of black carbon (BC) emissions on monsoon rainfall patterns across the Indian subcontinent. The results show that BC exerts localized warming effects, providing valuable insights into the mechanisms influencing the rainfall distribution across the Indian landmass. The study analyzes the vertical profile of mean tropospheric temperature differences between two sets of simulations: (i) with default BC emissions (WBC) and (ii) with BC emissions reduced by 99% (WoBC), conducted for JJAS, 2017, focusing on the region along the eastern coast. The analysis of the tropospheric temperature variations over the eastern coast reveals significant rainfall differences, primarily attributed to the intensification of convective rainfall. The results indicate that WoBC simulation leads to abnormal cooling in the lower troposphere and warming in the mid-upper troposphere, plausibly linked to the release of latent heat from the enhanced convective activity observed over the region. These alterations in the tropospheric temperature profile correspond remarkably well with the changes in the spatial distribution of rainfall over this area, providing valuable insights into the intricate dynamics of the climate system over this region

Operational Probabilistic Fog Prediction Based on Ensemble Forecast System: A Decision Support System for Fog

One of the well-known challenges of fog forecasting is the high spatio-temporal variability of fog. An ensemble forecast aims to capture this variability by representing the uncertainty in the initial/lateral boundary conditions (ICs/BCs) and model physics. The present study highlights a new operational Ensemble Forecast System (EFS) developed by the Indian Institute of Tropical Meteorology (IITM), Pune, to predict the fog over the Indo-Gangetic Plain (IGP) region using the visibility (Vis) diagnostic algorithm. The EFS framework comprises the WRF model with a 4 km horizontal resolution, initialized by 21 ICs/BCs. The advantages of probabilistic fog forecasting have been demonstrated by comparing control (CNTL) and ensemble-based fog forecasts. The forecast is verified using fog observations from the Indira Gandhi International (IGI) airport during the winter months of 2020–2021 and 2021–2022. The results show that with a probability threshold of 50%, the ensemble forecasts perform better than the CNTL forecasts. The skill scores of EFS are relatively promising, with a Hit Rate of 0.95 and a Critical Success Index of 0.55; additionally, the False Alarm Rate and Missing Rate are low, with values of 0.43 and 0.04, respectively. The EFS could correctly predict more fog events (37 out of 39) compared with the CNTL forecast (31 out of 39) and shows the potential skill. Furthermore, EFS has a substantially reduced error in predicting fog onset and dissipation (mean onset and dissipation error of 1 h each) compared to the CNTL forecasts

Operational Probabilistic Fog Prediction Based on Ensemble Forecast System: A Decision Support System for Fog

One of the well-known challenges of fog forecasting is the high spatio-temporal variability of fog. An ensemble forecast aims to capture this variability by representing the uncertainty in the initial/lateral boundary conditions (ICs/BCs) and model physics. The present study highlights a new operational Ensemble Forecast System (EFS) developed by the Indian Institute of Tropical Meteorology (IITM), Pune, to predict the fog over the Indo-Gangetic Plain (IGP) region using the visibility (Vis) diagnostic algorithm. The EFS framework comprises the WRF model with a 4 km horizontal resolution, initialized by 21 ICs/BCs. The advantages of probabilistic fog forecasting have been demonstrated by comparing control (CNTL) and ensemble-based fog forecasts. The forecast is verified using fog observations from the Indira Gandhi International (IGI) airport during the winter months of 2020–2021 and 2021–2022. The results show that with a probability threshold of 50%, the ensemble forecasts perform better than the CNTL forecasts. The skill scores of EFS are relatively promising, with a Hit Rate of 0.95 and a Critical Success Index of 0.55; additionally, the False Alarm Rate and Missing Rate are low, with values of 0.43 and 0.04, respectively. The EFS could correctly predict more fog events (37 out of 39) compared with the CNTL forecast (31 out of 39) and shows the potential skill. Furthermore, EFS has a substantially reduced error in predicting fog onset and dissipation (mean onset and dissipation error of 1 h each) compared to the CNTL forecasts

Thermodynamical framework for effective mitigation of high aerosol loading in the Indo-Gangetic Plain during winter

Abstract The Indo-Gangetic Plain (IGP) experiences severe air pollution every winter, with ammonium chloride and ammonium nitrate as the major inorganic fractions of fine aerosols. Many past attempts to tackle air pollution in the IGP were inadequate, as they targeted a subset of the primary pollutants in an environment where the majority of the particulate matter burden is secondary in nature. Here, we provide new mechanistic insight into aerosol mitigation by integrating the ISORROPIA-II thermodynamical model with high-resolution simultaneous measurements of precursor gases and aerosols. A mathematical framework is explored to investigate the complex interaction between hydrochloric acid (HCl), nitrogen oxides (NOx), ammonia (NH3), and aerosol liquid water content (ALWC). Aerosol acidity (pH) and ALWC emerge as governing factors that modulate the gas-to-particle phase partitioning and mass loading of fine aerosols. Six "sensitivity regimes" were defined, where PM1 and PM2.5 fall in the "HCl and HNO3 sensitive regime", emphasizing that HCl and HNO3 reductions would be the most effective pathway for aerosol mitigation in the IGP, which is ammonia-rich during winter. This study provides evidence that precursor abatement for aerosol mitigation should not be based on their descending mass concentrations but instead on their sensitivity to high aerosol loading