New Particle Formation in the Atmosphere: From Molecular Clusters to Global Climate

Journal of Geophysical Research Atmospheres, Год журнала: 2019, Номер 124(13), С. 7098 - 7146

Опубликована: Июнь 25, 2019

Abstract New particle formation (NPF) represents the first step in complex processes leading to of cloud condensation nuclei. Newly formed nanoparticles affect human health, air quality, weather, and climate. This review provides a brief history, synthesizes recent significant progresses, outlines challenges future directions for research relevant NPF. developments include emergence state‐of‐the‐art instruments that measure prenucleation clusters newly nucleated down about 1 nm; systematic laboratory studies multicomponent nucleation systems, including collaborative experiments conducted Cosmics Leaving Outdoor Droplets chamber at CERN; observations NPF different types forests, extremely polluted urban locations, coastal sites, polar regions, high‐elevation sites; improved theories parameterizations account atmospheric models. The lack understanding fundamental chemical mechanisms responsible aerosol growth under diverse environments, effects SO 2 NO x on NPF, contribution anthropogenic organic compounds It is also critical develop can detect composition particles from 3 20 nm improve represent over wide range conditions precursor, temperature, humidity.

Язык: Английский

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Differing Mechanisms of New Particle Formation at Two Arctic Sites

Geophysical Research Letters, Год журнала: 2020, Номер 48(4)

Опубликована: Дек. 29, 2020

Abstract New particle formation in the Arctic atmosphere is an important source of aerosol particles. Understanding processes secondary crucial due to their significant impact on cloud properties and therefore amplification. We observed molecular new particles from low‐volatility vapors at two sites with differing surroundings. In Svalbard, sulfuric acid (SA) methane sulfonic (MSA) contribute some extent condensation nuclei (CCN). This occurs via ion‐induced nucleation SA NH 3 subsequent growth by mainly MSA during springtime highly oxygenated organic molecules summertime. By contrast, ice‐covered region around Villum, we driven iodic but its concentration was insufficient grow nucleated CCN sizes. Our results provide insight about sources precursors

Язык: Английский

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Role of iodine oxoacids in atmospheric aerosol nucleation

Science, Год журнала: 2021, Номер 371(6529), С. 589 - 595

Опубликована: Фев. 4, 2021

Faster than expected Iodine species are one of only a handful atmospheric vapors known to make new aerosol particles, which play central role in controlling the radiative forcing climate. He et al. report experimental evidence from CERN Cosmics Leaving Outdoor Droplets, or CLOUD, chamber demonstrating that iodic acid and iodous rapidly form particles can compete with sulfuric pristine regions. Science , this issue p. 589

Язык: Английский

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Overview of the Antarctic Circumnavigation Expedition: Study of Preindustrial-like Aerosols and Their Climate Effects (ACE-SPACE)

Bulletin of the American Meteorological Society, Год журнала: 2019, Номер 100(11), С. 2260 - 2283

Опубликована: Июль 2, 2019

Abstract Uncertainty in radiative forcing caused by aerosol–cloud interactions is about twice as large for CO 2 and remains the least well understood anthropogenic contribution to climate change. A major cause of uncertainty poorly quantified state aerosols pristine preindustrial atmosphere, which defines baseline against effects are calculated. The Southern Ocean one few remaining near-pristine aerosol environments on Earth, but there very measurements help evaluate models. Antarctic Circumnavigation Expedition: Study Preindustrial-like Aerosols their Climate Effects (ACE-SPACE) took place between December 2016 March 2017 covered entire region (Indian, Pacific, Atlantic Oceans; length ship track >33,000 km) including previously unexplored areas. In situ characteristics [e.g., chemical composition, size distributions, cloud condensation nuclei (CCN) number concentrations], trace gases, meteorological variables. Remote sensing observations properties, physical microbial ocean state, back trajectory analyses used interpret data. sea spray CCN westerly wind belt can be larger than 50%. abundance methanesulfonic acid indicates local regional influence coastal waters open ocean. We use data simulated concentrations from a global model. extensive, available ACE-SPACE dataset ( https://zenodo.org/communities/spi-ace?page=1&size=20 ) provides an unprecedented opportunity models reduce associated with natural processes emission, formation, transport, processing occurring over Ocean.

Язык: Английский

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Sulfuric acid–amine nucleation in urban Beijing

Atmospheric chemistry and physics, Год журнала: 2021, Номер 21(4), С. 2457 - 2468

Опубликована: Фев. 18, 2021

Abstract. New particle formation (NPF) is one of the major sources atmospheric ultrafine particles. Due to high aerosol and trace gas concentrations, mechanism governing factors for NPF in polluted boundary layer may be quite different from those clean environments, which however less understood. Herein, based on long-term measurements January 2018 March 2019 Beijing, nucleation influences H2SO4 concentration, amine concentration are quantified. The collision H2SO4–amine clusters found dominating initialize urban Beijing. coagulation scavenging due a factor as it limits new rates. Beijing sometimes limited by low concentrations. Summarizing synergistic effects we elucidate various conditions.

Язык: Английский

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Open ocean and coastal new particle formation from sulfuric acid and amines around the Antarctic Peninsula

Nature Geoscience, Год журнала: 2021, Номер 14(6), С. 383 - 388

Опубликована: Май 13, 2021

Язык: Английский

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Enhanced growth rate of atmospheric particles from sulfuric acid

Atmospheric chemistry and physics, Год журнала: 2020, Номер 20(12), С. 7359 - 7372

Опубликована: Июнь 25, 2020

Abstract. In the present-day atmosphere, sulfuric acid is most important vapour for aerosol particle formation and initial growth. However, growth rates of nanoparticles (<10 nm) from remain poorly measured. Therefore, effect stabilizing bases, contribution ions impact attractive forces on molecular collisions are under debate. Here, we present precise rate measurements uncharged particles 1.8 to 10 nm, performed atmospheric conditions in CERN (European Organization Nuclear Research) CLOUD chamber. Our results show that evaporation above 2 nm negligible, proceeds kinetically even at low ammonia concentrations. The experimental exceed hard-sphere kinetic limit condensation acid. We demonstrate this van der Waals between molecules disentangle it charge–dipole interactions. magnitude enhancement depends assumed hydration collision kinetics but increasingly smaller sizes, resulting a steep rise observed with decreasing size. Including global model, find enhanced increases predicted number concentrations upper free troposphere by more than 50 %.

Язык: Английский

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Simultaneous Detection of Alkylamines in the Surface Ocean and Atmosphere of the Antarctic Sympagic Environment

ACS Earth and Space Chemistry, Год журнала: 2019, Номер 3(5), С. 854 - 862

Опубликована: Апрель 5, 2019

Measurements of alkylamines from seawater and atmospheric samples collected simultaneously across the Antarctic Peninsula, South Orkney Georgia Islands are reported. Concentrations mono-, di-, trimethylamine (MMA, DMA, TMA, respectively), their precursors, quarternary amines glycine betaine choline, were enhanced in sympagic relative to ice-devoid pelagic ones, suggesting microbiota sea ice ice-influenced ocean is a major source these compounds. Primary sea-spray aerosol particles artificially generated by bubbling investigated time-of-flight mass spectrometry (ATOFMS) single particles; mixing state indicated that aerosolized with spray dissolved particulate organic nitrogen pools. Despite this unequivocal spray-associated alkylamines, ATOFMS analyses ambient aerosols region majority (75–89%) secondary origin, is, incorporated into after gaseous air–sea exchange. These findings show properties influencing biogenic fluxed boundary layer; compounds should be considered when assessing formation processes Antarctica.

Язык: Английский

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Atmospheric Sulfuric Acid‐Dimethylamine Nucleation Enhanced by Trifluoroacetic Acid

Geophysical Research Letters, Год журнала: 2020, Номер 47(2)

Опубликована: Янв. 8, 2020

Abstract Sulfuric acid (SA)‐dimethylamine (DMA)‐H 2 O cluster formation has been proven to be responsible for a significant part of new particle (NPF) in Chinese megacity. However, the possible involvement common atmospheric acids subsequent growth SA‐DMA clusters remains elusive. We simulated and using relevant concentrations SA, DMA, trifluoroacetic (TFA), commonly observed perfluorocarboxylic acid, Density Functional Theory combined with Atmospheric Cluster Dynamics Code. The presence TFA leads complex routes an enhancement NPF rates by up 2.3 ([TFA] = 5.0 × 10 6 molecules cm −3 , [SA] 1.0 [DMA] 1.5 9 ). agreement (SA) 1 ·(DMA) 1‐2 ·(TFA) between simulations ambient measurements during events validates model predictions implies that could potentially boost rates.

Язык: Английский

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Acid–Base Clusters during Atmospheric New Particle Formation in Urban Beijing

Environmental Science & Technology, Год журнала: 2021, Номер 55(16), С. 10994 - 11005

Опубликована: Авг. 2, 2021

Molecular clustering is the initial step of atmospheric new particle formation (NPF) that generates numerous secondary particles. Using two online mass spectrometers with and without a chemical ionization inlet, we characterized neutral clusters naturally charged ion during NPF periods in urban Beijing. In clusters, observed pure sulfuric acid (SA) SA-amine SA-ammonia (NH

Язык: Английский

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