The Indo-Gangetic Plain (IGP) is one of the dominant sources of air pollution worldwide. During winter, the variations in planetary boundary layer (PBL) height, driven by a strong radiative thermal inversion, affect the regional air pollution dispersion. To date, measurements of aerosol-water vapour interactions, especially cloud condensation nuclei (CCN) activity, are limited in the Indian sub-continent, causing large uncertainties in the radiative forcing estimates of aerosol-cloud interactions. We present the results of a one-month field campaign (February-March 2018) in the megacity, Delhi, a significant polluter in the IGP. We measured the composition of fine particulate matter (PM1) and size-resolved CCN properties over a wide range of water vapour supersaturations. The analysis includes PBL modelling, backward trajectories, and fire spots to elucidate the influence of PBL and air mass origins on the aerosols. The aerosol properties depended strongly on the PBL height, and a simple power-law fit could parameterize the observed correlations of PM1 mass, aerosol particle number, and CCN number with PBL height, indicating PBL induced changes in aerosol accumulation. The low inorganic mass fractions, low aerosol hygroscopicity and high externally mixed weakly CCN-active particles under low PBL height (<100 m) indicated the influence of the PBL on aerosol aging processes. In contrast, aerosol properties did not depend strongly on air mass origins or wind direction, implying that the observed aerosol and CCN are from local emissions. An error function could parameterize the relationship between CCN number and supersaturation throughout the campaign.

Our abilities to predict the extent and impacts of atmospheric black carbon depend on the accuracy of inventories, which are known to be highly uncertain in the developing world. This is because of less regulation of industry and vehicles, the private use of lower-quality fuels and appliances and a lack of data on activity. In order to provide better constraint on emissions from a developing megacity, the fluxes of refractory black carbon were measured using a Single Particle Soot Photometer (SP2) and the eddy covariance method, which is a relatively new technique. These were made on top of a purpose-built tower alongside a suite of other aerosol and gas flux measurements as part of the NERC/Newton Fund ‘DelhiFlux’ project, part of the Air Pollution and Human Health (APHH) Delhi programme. The location was the campus of the Indira Gandhi Delhi Technical University for Women (IGDTUW) in Old Delhi, where emissions were deemed to be representative of the less economically developed areas of the city. Statistically significant rBC mass fluxes of around 10-30 ng m-2 s-1 were measured and these were strongest in the morning. The rBC particles observed could be categorised into distinct types according to their coating thicknesses according to the SP2 Leading Edge Only (LEO) method, however unlike previously published observations in London and Beijing, no clear sources could be attributed to the different coating types. Through comparisons with other measurements such as NOx and AMS factorisation, it appears that the main sector responsible for rBC emissions in the area is transport, which is consistent with the SAFAR inventory, although cooking also seemed to contribute. However, the magnitude and diurnal profile of the measured emissions differed significantly from the inventory, with the measurements being lower by a factor of 50-60 and peaking earlier in the day.

Covid lockdown presented an important opportunity to study relatively cleaner conditions in India. The complex factors of power production, industry, and transportation could be more carefully dissected because of the extreme reduction in the influence of the latter two emission sources. Measurements of cloud condensation nuclei (CCN) activity and other chemical properties of atmospheric aerosols showed that newly formed aerosol particles were produced in the SO2 plume from a large coal-fired power plant, contrary to normal conditions of heavy pollution. The sulfate-rich particles had high CCN activity and number concentration, indicating high cloud-forming potential. Examining the sensitivity of CCN properties under relatively clean conditions over India provides important new constraints on the perturbations of past and future climate forcing by anthropogenic emissions. Because most sensitive regime of aerosol climate forcing on cloud development is the midpoint of relatively clean conditions afforded by the Covid lockdown between background and polluted conditions.

The science guiding the \EURECA campaign and its measurements are presented. \EURECA comprised roughly five weeks of measurements in the downstream winter trades of the North Atlantic — eastward and south-eastward of Barbados. Through its ability to characterize processes operating across a wide range of scales, \EURECA marked a turning point in our ability to observationally study factors influencing clouds in the trades, how they will respond to warming, and their link to other components of the earth system, such as upper-ocean processes or, or the life-cycle of particulate matter. This characterization was made possible by thousands (2500) of sondes distributed to measure circulations on meso (200 km) and larger (500 km) scales, roughly four hundred hours of flight time by four heavily instrumented research aircraft, four global-ocean class research vessels, an advanced ground-based cloud observatory, a flotilla of autonomous or tethered measurement devices operating in the upper ocean (nearly 10000 profiles), lower atmosphere (continuous profiling), and along the air-sea interface, a network of water stable isotopologue measurements, complemented by special programmes of satellite remote sensing and modeling with a new generation of weather/climate models. In addition to providing an outline of the novel measurements and their composition into a unified and coordinated campaign, the six distinct scientific facets that \EURECA explored — from Brazil Ring Current Eddies to turbulence induced clustering of cloud droplets and its influence on warm-rain formation — are presented along with an overview \EURECA’s outreach activities, environmental impact, and guidelines for scientific practice.

The southeast Atlantic Ocean provides an excellent natural laboratory to study smoke-cloud interactions, a large driver of uncertainty in climate projections. The value of studying this in particular region is largely attributable to two factors---the expansive, bright, semi-permanent stratocumulus cloud deck and the fact that southern Africa is the largest source of biomass-burning aerosols in the world. We study this region using the WRF-Chem model with CAM5 aerosols and in situ observations from the ORACLES, LASIC, and CLARIFY field campaigns, all of which overlapped in August 2017. Across these campaigns, we compare aerosol, cloud, and thermodynamic variables to quantify model performance and expand upon observational findings of aerosol-cloud effects. Specifically, our approach is to analyze aerosol and cloud properties along flight tracks, picking out uniform legs within tropospheric smoke plumes and in the boundary layer. This unique approach allows us to sample the high spatiotemporal variability that can get lost to large-scale averaging. It also allows process-level comparison of local cloud responses to aerosol conditions, and measure model performance in those same processes. Along with better quantifying model predictive power, we find and justify updates to model parameters and processes to better emulate observations, notably aerosol size parameters. Preliminary results suggest that WRF-CAM5 is activating a smaller percentage of aerosols into cloud droplets than shown in observations, which could lead to biased modeling of aerosol indirect radiative effects on a larger scale. We explore this effect further with CCN activation tendency, updraft, particle sizing, and composition analysis, as well as broader dynamics like entrainment and removal rates. Comparing the model with similar instrument suites across multiple colocated campaigns also allows us to quantify instrument uncertainty in ways that a focus on a single campaign cannot and gives further context to the model performance.

Biomass-burning emissions impact almost all of the radiative forcing terms considered by the IPCC, yet little is known about smoke aerosol aging in nature beyond a few days. The marine southeast Atlantic free-troposphere is a natural testbed for examining aging through photolysis/oxidation of African continental fire emissions advected westward. In-situ measurements primarily from September, 2016 indicate highly-oxidized aerosol with minimal primary source signatures after 4-9 model-predicted days since emission. Aerosol loses approximately one-half of its organic aerosol over the ocean. The organic aerosol to black carbon mass ratios decrease from 14 to 10, significantly lower than many model predictions. This mass loss, combined with stability in black carbon, supports an observed 20% increase in solar absorptivity. The decreased single scattering albedos, reaching 0.83 at 9 days, arguably represent the lowest values measured globally. The relationship of the aerosol properties to model-derived time since emission suggests a useful new modeling constraint.