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It is well known that atmospheric aerosol size and composition impact air quality, climate, and health. The aerosol composition is typically a mixture and consists of a wide range of organic and inorganic particles that interact with each other. Furthermore, water vapor is ubiquitous in the atmosphere, in indoor air, and within the human body’s respiratory system, and the presence of water can alter the aerosol morphology and propensity to form droplets. Specifically, aerosol mixtures can undergo liquid–liquid phase separation (LLPS) in the presence of water vapor. However, the experimental conditions for which LLPS impacts water uptake and the subsequent prediction of aerosol mixtures are poorly understood. To improve our understanding of aerosol mixtures and droplets, this study explores two ternary systems that undergo LLPS, namely, the 2MGA system (sucrose + ammonium sulfate + 2-methylglutaric acid) and the PEG1000 system (sucrose + ammonium sulfate + polyethylene glycol 1000). In this study, the ratio of species and the O:C ratios are systematically changed, and the hygroscopic properties of the resultant aerosol were investigated. Here, we show that the droplet activation above 100% RH of the 2MGA system was influenced by LLPS, while the droplet activation of the PEG1000 system was observed to be linearly additive regardless of chemical composition, O:C ratio, and LLPS. A theoretical model that accounts for LLPS with O:C ratios was developed and predicts the water uptake of internally mixed systems of different compositions and phase states. Hence, this study provides a computationally efficient algorithm to account for the LLPS and solubility parameterized by the O:C ratio for droplet activation at supersaturated relative humidity conditions and may thus be extended to mixed inorganic–organic aerosol populations with unspeciated organic composition found in the ambient environment.more » « less
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null (Ed.)Ambient temperature and humidity strongly affect inactivation rates of enveloped viruses, but a mechanistic, quantitative theory of these effects has been elusive. We measure the stability of SARS-CoV-2 on an inert surface at nine temperature and humidity conditions and develop a mechanistic model to explain and predict how temperature and humidity alter virus inactivation. We find SARS-CoV-2 survives longest at low temperatures and extreme relative humidities (RH); median estimated virus half-life is >24 hours at 10C and 40% RH, but ~1.5 hours at 27C and 65% RH. Our mechanistic model uses fundamental chemistry to explain why inactivation rate increases with increased temperature and shows a U-shaped dependence on RH. The model accurately predicts existing measurements of five different human coronaviruses, suggesting that shared mechanisms may affect stability for many viruses. The results indicate scenarios of high transmission risk, point to mitigation strategies, and advance the mechanistic study of virus transmission.more » « less
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4-Mercaptopyridine (4-Mpy) is a pH reporter molecule commonly used to functionalize nanoprobes for surface-enhanced Raman spectroscopy (SERS) based pH measurements. However, nanoprobes functionalized by 4-Mpy alone have low pH sensitivity and are subject to interference by halide ions in sample media. To improve nanoprobe pH sensitivity and reliability, we functionalized gold nanoparticles (AuNPs) with both 4-Mpy and bromide ion (Br − ). Br − electrostatically stabilizes protonated 4-Mpy, thus enabling sensitive SERS detection of the protonation state of 4-Mpy as a function of pH while also reducing variability caused by external halide ions. Through optimization of the functionalization parameters, including suspension pH, [4-Mpy], and [Br − ], the developed nanoprobes enable monitoring of pH from 2.1 to 10 with high SERS activity and minimal interference from halide ions within the sample matrix. As a proof of concept, we were able to track nanoprobe location and image the pH distribution inside individual cancer cells. This study provides a novel way to engineer reliable 4-Mpy-functionalized SERS nanoprobes for the sensitive analysis of spatially localized pH features in halide ion-containing microenvironments.more » « less
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