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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.

Ice-nucleating particles (INPs) are crucial for cloud freezing processes in the atmosphere. Given the limited knowledge about the vertical distribution of INPs and its relation to aerosols in China, we present two aircraft observations of INPs over the North China Plain on 23 October 2019 and 25 October 2019, before and after a cold front passage. We used a well-established method to identify the INPs on a silicon wafer and then performed single-particle chemical composition analysis using an environmental scanning electron microscope-energy dispersive spectrometer (ESEM-EDS). The INP concentrations range from 0.1 to 9.2 L−1 within activation temperatures from −20 to −29 °C. INPs are mostly concentrated within the boundary layer, and their concentration shows a decreasing trend with height (0.5~6 km) before the cold front passage. However, the highest INP concentration always appears at higher altitudes (4~5 km) after the cold front passage. The cold front passage also significantly weakens the correlations between the concentrations of INPs and aerosol particles at different sizes. The activated fraction (AF) of total aerosols increases from 10−6 to 10−4 with height from near ground to 6 km, reflecting a better nucleating capacity of the aerosols at higher altitudes. There is no obvious variation in AF after the cold front passage. Chemical analysis reveals that the INPs containing mineral dust components comprise the majority of total INPs during both flights. The proportion of pure mineral dust declines from 52.2% to 43.5% after the cold front passage while the proportion of mixed mineral dust increases from 23.9% to 45.7%, suggesting that an increased probability of aging or coating of INPs is introduced by the cold front during their long-distance transport. In addition, 88% of INPs have a diameter larger than 1 μm. This indicates that larger aerosols (>1 μm) are the major contributors to INPs at high altitudes despite their relatively low abundance. Our results demonstrate a significant impact of transport events on the sources and vertical distribution of INPs in the atmosphere.

The Neckar Valley and the Swabian Jura in southwest Germany comprise a hotspot for severe convective storms, causing tens of millions of euros in damage each year. Possible reasons for the high frequency of thunderstorms and the associated event chain across compartments were investigated in detail during the hydro-meteorological field campaign Swabian MOSES carried out between May and September 2021. Researchers from various disciplines established more than 25 temporary ground-based stations equipped with state-of-the-art in situ and remote sensing observation systems, such as lidars, dual-polarization X- and C-band Doppler weather radars, radiosondes including stratospheric balloons, an aerosol cloud chamber, masts to measure vertical fluxes, autosamplers for water probes in rivers, and networks of disdrometers, soil moisture, and hail sensors. These fixed-site observations were supplemented by mobile observation systems, such as a research aircraft with scanning Doppler lidar, a cosmic ray neutron sensing rover, and a storm chasing team launching swarmsondes in the vicinity of hailstorms. Seven Intensive Observation Periods (IOPs) were conducted on a total of 21 operating days. An exceptionally high number of convective events, including both unorganized and organized thunderstorms such as multicells or supercells, occurred during the study period. This paper gives an overview of the Swabian MOSES (Modular Observation Solutions for Earth Systems) field campaign, briefly describes the observation strategy, and presents observational highlights for two IOPs.

The aerosol chamber AIDA (Aerosol Interactions and Dynamics in the Atmosphere) was used as a moderate expansion cloud chamber to investigate the effect of the organic carbon (OC) content on the ice nucleation properties of soot aerosol particles. Two different soot samples with OC contents of 16 % (CS16) and 40 % (CS40) where produced with the CAST (Combustion Aerosol Standard) burner operated at different air/fuel (propane) ratios. In dynamic expansion experiments with about 30 %/min increase of relative humidity with respect to ice, the CS16 sample started to nucleate ice crystals at an ice saturation ratio Sin of 1.45 (at a temperature of 207 K). This value is very close to the ice saturation ratio of ice nucleation onset on carbon spark generator soot particles coated with a significant amount of sulphuric acid investigated in previous AIDA expansion experiments. A second experiment with CS40 soot performed at almost identical thermodynamic conditions showed ice nucleation onset to occur at Sin between 1.5 and 1.7. The formation rate of ice crystals was at least two orders of magnitude less than for CS16 soot, even at ice saturation ratios up to values of 1.9, which is very close to water saturation at a temperature of 207 K. Therefore, increasing the amount of OC seems to significantly suppress the ice nucleation on flame soot particles. In contrast, similar expansion experiments with dry and untreated mineral dust particles (Arizona test dust) in the temperature range 194 to 241 K showed ice nucleation to occur at much lower ice saturation ratios of only 1.05 to 1.15.

The aerosol chamber AIDA was used as a moderate expansion cloud chamber with cooling rates at the onset of ice nucleation between -1.3 and -3.0 K min−1 to investigate the nucleation and growth of ice crystals in sulphuric acid, ammonium sulphate, and mineral dust aerosols at temperatures between 196 and 224 K. Supercooled sulphuric acid droplets with mean diameters of about 0.2 to 0.3 μm nucleated ice by homogeneous freezing at RHice increasing from 144 to 166 % with temperatures from 220 and 196 K. This is in good agreement both with previous results of AIDA experiments and literature data. In contrast, ammonium sulphate particles of similar size nucleated ice at the significantly lower RHice of 120 to 127 % in the same temperature range. Fourier-Transform infrared (FTIR) extinction spectra of the aerosol revealed that the ammonium sulphate particles, mainly consisted of the liquid phase. The number concentration of ice crystals formed during the homogeneous freezing experiments agree well with model results from the literature. Higher ice crystal number concentrations formed during the ammonium sulphate, compared to the sulphuric acid experiments, can be explained by the also somewhat higher cooling rates at ice nucleation. Deposition ice nucleation on mineral dust particles turned out to be the most efficient ice nucleation mechanism both with respect to RHice at the onset of ice nucleation (102 to 105 % in the temperature range 209 to 224 K) and the ice crystal number concentration. Almost all mineral dust particles nucleated ice at the lower temperatures.