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  1. Abstract

    Transformation of low-volatility gaseous precursors to new particles affects aerosol number concentration, cloud formation and hence the climate. The clustering of acid and base molecules is a major mechanism driving fast nucleation and initial growth of new particles in the atmosphere. However, the acid–base cluster composition, measured using state-of-the-art mass spectrometers, cannot explain the measured high formation rate of new particles. Here we present strong evidence for the existence of base molecules such as amines in the smallest atmospheric sulfuric acid clusters prior to their detection by mass spectrometers. We demonstrate that forming (H2SO4)1(amine)1 is the rate-limiting step in atmospheric H2SO4-amine nucleation and the uptake of (H2SO4)1(amine)1 is a major pathway for the initial growth of H2SO4 clusters. The proposed mechanism is very consistent with measured new particle formation in urban Beijing, in which dimethylamine is the key base for H2SO4 nucleation while other bases such as ammonia may contribute to the growth of larger clusters. Our findings further underline the fact that strong amines, even at low concentrations and when undetected in the smallest clusters, can be crucial to particle formation in the planetary boundary layer.

     
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  2. Abstract

    Understanding the formation processes of particles and cloud condensation nuclei (CCN) in pristine environments is a major challenge in assessing the anthropogenic impacts on climate change. Using a state‐of‐the‐art model that systematically simulates the new‐particle formation (NPF) from condensable vapors and multi‐scale transport of chemical species, we find that NPF contributes ∼90% of the particle number and ∼80% of the CCN at 0.5% supersaturation (CCN0.5%) in the pristine Amazon boundary layer during the wet season. The corresponding contributions are only ∼30% and ∼20% during the dry season because of prevalent biomass burning. In both seasons, ∼50% of the NPF‐induced particles and ∼85% of the NPF‐induced CCN0.5% in the boundary layer originate from the long‐range transport of new particles formed hundreds to thousands of kilometers away. Moreover, about 50%–65% of the NPF‐induced particles and 35%–50% of the NPF‐induced CCN0.5% originate from the downward transport of new particles formed aloft.

     
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  3. The main nucleating vapor in the atmosphere is thought to be sulfuric acid (H2SO4), stabilized by ammonia (NH3). However, in marine and polar regions, NH3is generally low, and H2SO4is frequently found together with iodine oxoacids [HIOx, i.e., iodic acid (HIO3) and iodous acid (HIO2)]. In experiments performed with the CERN CLOUD (Cosmics Leaving OUtdoor Droplets) chamber, we investigated the interplay of H2SO4and HIOxduring atmospheric particle nucleation. We found that HIOxgreatly enhances H2SO4(-NH3) nucleation through two different interactions. First, HIO3strongly binds with H2SO4in charged clusters so they drive particle nucleation synergistically. Second, HIO2substitutes for NH3, forming strongly bound H2SO4-HIO2acid-base pairs in molecular clusters. Global observations imply that HIOxis enhancing H2SO4(-NH3) nucleation rates 10- to 10,000-fold in marine and polar regions.

     
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    Free, publicly-accessible full text available December 15, 2024
  4. Abstract The interaction between nitrogen monoxide (NO) and organic peroxy radicals (RO 2 ) greatly impacts the formation of highly oxygenated organic molecules (HOM), the key precursors of secondary organic aerosols. It has been thought that HOM production can be significantly suppressed by NO even at low concentrations. Here, we perform dedicated experiments focusing on HOM formation from monoterpenes at low NO concentrations (0 – 82 pptv). We demonstrate that such low NO can enhance HOM production by modulating the RO 2 loss and favoring the formation of alkoxy radicals that can continue to autoxidize through isomerization. These insights suggest that HOM yields from typical boreal forest emissions can vary between 2.5%-6.5%, and HOM formation will not be completely inhibited even at high NO concentrations. Our findings challenge the notion that NO monotonically reduces HOM yields by extending the knowledge of RO 2 -NO interactions to the low-NO regime. This represents a major advance towards an accurate assessment of HOM budgets, especially in low-NO environments, which prevails in the pre-industrial atmosphere, pristine areas, and the upper boundary layer. 
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    Free, publicly-accessible full text available December 1, 2024
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  7. Free, publicly-accessible full text available September 26, 2024