Search for: All records

Abstract During summer, ammonia emissions in Southeast Asia influence air pollution and cloud formation. Convective transport by the South Asian monsoon carries these pollutant air masses into the upper troposphere and lower stratosphere (UTLS), where they accumulate under anticyclonic flow conditions. This air mass accumulation is thought to contribute to particle formation and the development of the Asian Tropopause Aerosol Layer (ATAL). Despite the known influence of ammonia and particulate ammonium on air pollution, a comprehensive understanding of the ATAL is lacking. In this modelling study, the influence of ammonia on particle formation is assessed with emphasis on the ATAL. We use the EMAC chemistry-climate model, incorporating new particle formation parameterisations derived from experiments at the CERN CLOUD chamber. Our diurnal cycle analysis confirms that new particle formation mainly occurs during daylight, with a 10-fold enhancement in rate. This increase is prominent in the South Asian monsoon UTLS, where deep convection introduces high ammonia levels from the boundary layer, compared to a baseline scenario without ammonia. Our model simulations reveal that this ammonia-driven particle formation and growth contributes to an increase of up to 80% in cloud condensation nuclei (CCN) concentrations at cloud-forming heights in the South Asian monsoon region. We find that ammonia profoundly influences the aerosol mass and composition in the ATAL through particle growth, as indicated by an order of magnitude increase in nitrate levels linked to ammonia emissions. However, the effect of ammonia-driven new particle formation on aerosol mass in the ATAL is relatively small. Ammonia emissions enhance the regional aerosol optical depth (AOD) for shortwave solar radiation by up to 70%. We conclude that ammonia has a pronounced effect on the ATAL development, composition, the regional AOD, and CCN concentrations. 

Abstract The Asian Summer Monsoon (ASM) convection transports aerosols and their precursors from the boundary layer to the upper troposphere and lower stratosphere (UTLS). This process forms an annually recurring aerosol layer near the tropopause. Recent observations have revealed a distinct property of the aerosol layer over the ASM region, it is nitrate‐rich. We present a newly implemented aerosol formation algorithm that enhances the representation of nitrate aerosol in the Community Aerosol and Radiation Model for Atmospheres (CARMA) coupled with the Community Earth System Model (CESM). The simulated aerosol chemical composition, as well as vertical distributions of aerosol size and mass, are evaluated using in situ and remote sensing observations. The simulated concentrations (ammonium, nitrate, and sulfate) and size distributions are generally within the error bars of data. We find nitrate, organics, and sulfate contribute significantly to the UTLS aerosol concentration between 15°–45°N and 0°–160°E. The two key formation mechanisms of nitrate‐containing aerosols in the ATAL are ammonium neutralization to form ammonium nitrate in regions where convection is active, and condensation of nitric acid in regions of cold temperature. Furthermore, including nitrate formation in the model doubles the surface area density in the tropical tropopause region between 15°–45°N and 0°–160°E, which alters the chlorine partitioning and subsequently impacts the rate of ozone depletion. 

Abstract Data collected with a holographic instrument [Holographic Detector for Clouds (HOLODEC)] on board the High-Performance Instrumented Airborne Platform for Environmental Research Gulfstream-V (HIAPER GV) aircraft from marine stratocumulus clouds during the Cloud System Evolution in the Trades (CSET) field project are examined for spatial uniformity. During one flight leg at 1190 m altitude, 1816 consecutive holograms were taken, which were approximately 40 m apart with individual hologram dimensions of 1.16 cm × 0.68 cm × 12.0 cm and with droplet concentrations of up to 500 cm−3. Unlike earlier studies, minimally intrusive data processing (e.g., bypassing calculation of number concentrations, binning, and parametric fitting) is used to test for spatial uniformity of clouds on intra- and interhologram spatial scales (a few centimeters and 40 m, respectively). As a means to test this, measured droplet count fluctuations are normalized with the expected standard deviation from theoretical Poisson distributions, which signifies randomness. Despite the absence of trends in the mean concentration, it is found that the null hypothesis of spatial uniformity on both spatial scales can be rejected with compelling statistical confidence. Monte Carlo simulations suggest that weak clustering explains this signature. These findings also hold for size-resolved analysis but with less certainty. Clustering of droplets caused by, for example, entrainment and turbulence, is size dependent and is likely to influence key processes such as droplet growth and thus cloud lifetime.