RESUMEN
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.
RESUMEN
The Indo-Gangetic Plain (IGP) has high wintertime fine aerosol loadings that significantly modulate the widespread fog formation and sustenance. Here, we investigate the potential formation of secondary inorganic aerosol driven by excess ammonia during winter fog. Physicochemical properties of fine aerosols (PM1 and PM2.5) and trace gases (HCl, HONO, HNO3, SO2, and NH3) were simultaneously monitored at hourly resolution using Monitor for AeRosols and Gases in Ambient air (MARGA-2S) for the first time in India. Results showed that four major ions, i.e., Cl-, NO3-, SO42-, and NH4+ contributed approximately 97% of the total measured inorganic ionic mass. The atmosphere was ammonia-rich in winter and ammonium was the dominant neutralizer with aerosol neutralization ratio (ANR) close to unity. The correlation between ammonium and chloride was ≥0.8, implying the significant formation of ammonium chloride during fog in Delhi. Thermodynamical model ISORROPIA-II showed the predicted PM1 and PM2.5 pH to be 4.49 ± 0.53, and 4.58 ± 0.48 respectively which were in good agreement with measurements. The ALWC increased from non-foggy to foggy periods and a considerable fraction of fine aerosol mass existed in the supermicron size range of 1-2.5 µm. The sulfur oxidation ratio (SOR) of PM1, PM2.5 reached up to 0.60, 0.75 in dense fog and 0.74, 0.87 when ambient RH crossed a threshold of 95%, much higher than non-foggy periods (with confidence level of ≥95%) pointing to enhanced formation of secondary aerosol in fog.
Asunto(s)
Contaminantes Atmosféricos , Material Particulado , Aerosoles/análisis , Contaminantes Atmosféricos/análisis , Amoníaco , Monitoreo del Ambiente , Material Particulado/análisis , Estaciones del AñoRESUMEN
The Middle East is one of the most water stressed regions in the world, receiving the majority of its hydrological input during the winter, in the form of highly variable and scattered precipitation. The persistence of wintertime anticyclonic conditions over the region can deflect storm tracks and result in extended spells of exceptionally hot weather, favoring prolonged droughts and posing a major threat to the already fragile hydrological equilibrium of the Middle East. Despite their potential impacts on water-security, winter warm spells (WWS's) have received far less attention than their summer counterparts, and the climatic drivers leading to WWS's onset are still largely unexplored. Here, we investigate their relationship with the internal modes of variability in the Atlantic Ocean, already known to influence winter circulation and extremes in Eurasia and Northern America. We show that the occurrence of WWS's is strongly correlated with Atlantic variability over decadal time scales. To explain this correlation, we propose a teleconnection mechanism linking Atlantic variability to WWS's via the propagation of Rossby waves from the North Atlantic pool, and the mediation of the Mediterranean circulation - thereby providing a basis to better predict future warming and aridification trends in the Middle East.