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Atmospheric aerosols exist as complex mixtures containing three or more compounds. Ternary aerosol mixtures composed of organic/organic/inorganic can undergo liquid–liquid phase separation (LLPS) under supersaturated conditions, affecting phase morphology and water uptake propensity. Phase separation and water uptake in ternary systems has previously been parameterized by oxygen to carbon (O[thin space (1/6-em)]:[thin space (1/6-em)]C) ratio; however, nitrogen containing organics, such as amino acid aerosols, also exist within complex mixtures. Yet, amino acid mixture CCN activity is poorly understood. In this study, we study the supersaturated hygroscopicity of three systems of internal mixtures containing ammonium sulfate (AS), 2-methylglutaric acid (2-MGA), and an amino acid. The three systems are AS/2-MGA/proline (Pro), AS/2-MGA/valine (Val), and AS/2-MGA/leucine (Leu). The amino acids are similar in O[thin space (1/6-em)]:[thin space (1/6-em)]C ratios but vary in solubility. Water-uptake, across a range of aerosol compositions in the ternary space, is measured using a cloud condensation nuclei counter (CCNC) from 0.4 to 1.7% supersaturation (SS). The single hygroscopicity parameter, κ, was calculated from CCNC measurements. All three systems exhibit two regions; one of these regions is phase separated mixtures when the composition is dominated by AS and 2-MGA; 2-MGA partitions to the droplet surface due to its surface-active nature and has a negligible contribution to water uptake. The second region is a homogeneous aerosol mixture, where all three compounds contribute to hygroscopicity. However, well mixed aerosol hygroscopicity is dependent on the solubility of the amino acid. Mixed Pro aerosols are the most hygroscopic while Leu aerosols are the least hygroscopic. Theoretical κ values were calculated using established models, including traditional κ-Köhler, O[thin space (1/6-em)]:[thin space (1/6-em)]C solubility and O[thin space (1/6-em)]:[thin space (1/6-em)]C-LLPS models. To account for the possible influence of polar N–C bonds on solubility and water uptake, the X[thin space (1/6-em)]:[thin space (1/6-em)]C parameterization is introduced through the X[thin space (1/6-em)]:[thin space (1/6-em)]C solubility and X[thin space (1/6-em)]:[thin space (1/6-em)]C-LLPS models; X[thin space (1/6-em)]:[thin space (1/6-em)]C is obtained from the ratio of oxygen and nitrogen to carbon. The study demonstrates competing organic–inorganic interactions driven by salting out effects in the presence of AS. Traditional methods cannot further encapsulate the non-ideal thermodynamic interactions within nitrogen-containing organic aerosol mixtures thus predictions of LLPS and hygroscopicity in nitrogen containing ternary systems should incorporate surface activity, O–C, N–C bonds, and salting out effects. 

Water vapor condensation on hygroscopic aerosol particles plays an important role in cloud formation, climate change, secondary aerosol formation, and aerosol aging. Conventional understanding considers deliquescence of nanosized hygroscopic aerosol particles a nearly instantaneous solid to liquid phase transition. However, the nanoscale dynamics of water condensation and aerosol particle dissolution prior to and during deliquescence remain obscure due to a lack of high spatial and temporal resolution single particle measurements. Here we use real time in situ transmission electron microscopy (TEM) imaging of individual sodium chloride (NaCl) nanoparticles to demonstrate that water adsorption and aerosol particle dissolution prior to and during deliquescence is a multistep dynamic process. Water condensation and aerosol particle dissolution was investigated for lab generated NaCl aerosols and found to occur in three distinct stages as a function of increasing RH. First, a < 100 nm water layer adsorbed on the NaCl cubes and caused sharp corners to dissolve and truncate. The water layer grew to several hundred nanometers with increasing RH and was rapidly saturated with solute, as evidenced by halting of particle dissolution. Adjacent cube corners displayed second-scale curvature fluctuations with no net particle dissolution or water layer thickness change. We propose that droplet solute concentration fluctuations drove NaCl transport from regions of high local curvature to regions of low curvature. Finally, we observed coexistence of a liquid water droplet and aerosol particle immediately prior to deliquescence. Particles dissolved discretely along single crystallographic directions, separating by few second lag times with no dissolution. This work demonstrates that deliquescence of simple pure salt particles with sizes in the range of 100 nm to several microns is not an instantaneous phase transition and instead involves a range of complex dissolution and water condensation dynamics. 

Abstract Air pollution in Africa is a significant public health issue responsible for 1.1 million premature deaths annually. Sub-Saharan Africa has the highest rate of population growth and urbanization of any region in the world, with substantial potential for future emission growth and worsening air quality. Accurate and extensive observations of meteorology and atmospheric composition have underpinned successful air pollution mitigation strategies in the Global North, yet Africa in general and East Africa in particular remain among the most sparsely observed regions in the world. This paper is based on the discussion of these issues during two international workshops, one held virtually in the United States in July 2021 and one in Kigali, Rwanda, in January 2023. The workshops were designed to develop a measurement, capacity building, and collaboration strategy to improve air quality-relevant measurements, modeling, and data availability in East Africa. This paper frames the relevant scientific needs and describes the requirements for training and infrastructure development for an integrated observing and modeling strategy that includes partnerships between East African scientists and organizations and their counterparts in the developed world.