Global variability in atmospheric new particle formation mechanisms

Nature, Journal Year: 2024, Volume and Issue: 631(8019), P. 98 - 105

Published: June 12, 2024

A key challenge in aerosol pollution studies and climate change assessment is to understand how atmospheric particles are initially formed

Language: Английский

---

Opinion: A paradigm shift in investigating the general characteristics of atmospheric new particle formation using field observations

Aerosol Research, Journal Year: 2024, Volume and Issue: 2(1), P. 49 - 58

Published: March 27, 2024

Abstract. Atmospheric new particle formation (NPF) and associated production of secondary particulate matter dominate aerosol number concentrations submicron mass loadings in many environments globally. Our recent investigations show that atmospheric NPF produces a significant amount particles on days when no clear event has been observed/identified. Furthermore, it observed different all around the world growth rates nucleation mode vary little, usually much less than measured condensable vapors. It also local clustering, which cases acts as starting point regional (NPF), can be described with intermediate ions at smallest sizes. These observations, together recently developed ranking method, lead us to propose paradigm shift investigations. In this opinion paper, we will summarize traditional approach describing describe an alternative covering both initial growth. The opportunities remaining challenges offered by are discussed.

Language: Английский

---

A cluster-of-functional-groups approach for studying organic enhanced atmospheric cluster formation

Aerosol Research, Journal Year: 2024, Volume and Issue: 2(1), P. 123 - 134

Published: June 4, 2024

Abstract. The role of organic compounds in atmospheric new particle formation is difficult to disentangle due the myriad potentially important oxygenated molecules (OOMs) present atmosphere. Using state-of-the-art quantum chemical methods, we here employ a novel approach, denoted “cluster-of-functional-groups” for studying involvement OOMs cluster formation. Instead usual “trial-and-error” approach testing ability experimentally identified form stable clusters with other nucleation precursors, study which, and how many, intermolecular interactions are required given OOM clusters. In this manner can reverse engineer elusive structure candidates that might be involved enhanced We calculated binding free energies all combinations donor acceptor functional groups investigate which most preferentially bind each precursors such as sulfuric acid bases (ammonia, methyl-, dimethyl- trimethylamine). find multiple carboxyl lead substantially more compared groups. Employing dynamics simulations, hypothetically composed stabilize acid–base provide recommendations potential multi-carboxylic tracer should explicitly studied future. presented generally applicable employed many applications, ion-induced elucidating structural patterns facilitate ice nucleation.

Language: Английский

---

The impact of ammonia on particle formation in the Asian Tropopause Aerosol Layer

npj Climate and Atmospheric Science, Journal Year: 2024, Volume and Issue: 7(1)

Published: Sept. 12, 2024

Language: Английский

---

Flame-Free Candles Are Not Pollution-Free: Scented Wax Melts as a Significant Source of Atmospheric Nanoparticles

Environmental Science & Technology Letters, Journal Year: 2025, Volume and Issue: 12(2), P. 175 - 182

Published: Feb. 3, 2025

Scented wax melts are being popularized as a safer, nontoxic alternative to traditional candles and incense for indoor aromatherapy. We performed field measurements in residential test house investigate atmospheric nanoparticle formation from scented melt use. employed high-resolution particle size magnifier-scanning mobility sizer (PSMPS) proton transfer reaction time-of-flight mass spectrometer (PTR-TOF-MS) real-time monitoring of distributions terpene mixing ratios, respectively. Our findings reveal that terpenes released react with ozone (O3) initiate new (NPF) events, resulting significant concentrations (>106 cm–3) comparable those emitted by combustion-based candles, gas stoves, diesel engines, natural engines. show melt-initiated NPF events can result respiratory exposures, tract deposited dose rates similar determined sources. results challenge the perception safer aromatherapy, highlighting need further research on toxicological properties newly formed nanoparticles better understand their environmental health implications.

Language: Английский

---

Elucidating New Particle Formation in Complex Terrain During the Winter 2022 Cold Fog Amongst Complex Terrain (CFACT) Campaign

Journal of Geophysical Research Atmospheres, Journal Year: 2025, Volume and Issue: 130(8)

Published: April 12, 2025

Abstract New particle formation (NPF) is a complex atmospheric phenomenon defined by the gas‐to‐particle conversion that leads to sudden burst and growth in aerosol particles. Although chemical mechanisms for nucleation are well established, role of physical processes, such as turbulent mixing, within boundary layer (ABL) beginning emerge with recent studies. This study, based on observations from 2022 CFACT (Cold Fog Amongst Complex Terrain) field study Heber Valley northern Utah, demonstrates an interconnection between turbulence occurrence NPF. Using spatially distributed instrumentation, novel feature CFACT, three case studies depict unique conditions modulate development NPF characterized sustained weak intermittent turbulence. Quantitative analysis using situ measurements derived variables demonstrate periods hinder growth, whereas helps These findings provide new insights into drivers NPF, underscoring impacting ABL.

Language: Английский

---

Quaternary Nucleation of Iodine and Sulfur Oxoacids in the Marine Atmosphere: Unexpected Role of Methanesulfonic Acid

Journal of Geophysical Research Atmospheres, Journal Year: 2025, Volume and Issue: 130(8)

Published: April 17, 2025

Abstract Sulfuric acid (SA), methanesulfonic (MSA), iodic (HIO 3 ), and iodous 2 ) are identified as key nucleation precursors can coexist in the marine atmosphere. Here, we investigated potential SA‐MSA‐HIO ‐HIO quaternary mechanism by exploring formation of (SA) w (MSA) x y z (0 ≤ + 3, 1 3) clusters with quantum chemical calculation kinetics modelling. The results indicate that effectively nucleate under atmospheric conditions. rate is up to 7 orders magnitude higher than SA/MSA‐HIO , ternary mechanisms, SA/MSA/HIO binary mechanisms at some specific mainly driven acid‐base reaction base) halogen bonds besides hydrogen bonds, three acids showing both competitive cooperative roles. More importantly, it was found contribution MSA aerosol comparable SA equal concentrations. unexpectedly high attributed its halogen‐bonding capacity SA. This study highlights need consider multicomponent atmosphere for accurate climate projections, may serve important proof weak even coexisting

Language: Английский

---

Automated Method for the Sensitive Analysis of Volatile Amines in Seawater

ACS ES&T Water, Journal Year: 2024, Volume and Issue: 4(6), P. 2504 - 2510

Published: May 3, 2024

Methylamines are polar, volatile, and organic nitrogen-containing compounds. They challenging to analyze, limiting our understanding of their occurrence role within the marine nitrogen cycle. We describe an automated headspace solid-phase microextraction method, coupled with gas chromatography phosphorus detection (HS-SPME-GC-NPD), for analyzing methylamines in seawater. Three SPME conditions were investigated: temperature, equilibration, extraction. The method was 6–24 times more sensitive trimethylamine (TMA) than dimethylamine (DMA) monomethylamine (MMA). DMA TMA detected small seawater volumes (2.5–10 mL), at 100–400 that previously reported. Detection limits 19.1, 6.6, 4.1 nM (nMol L–1) MMA, DMA, TMA, respectively, measured 10 mL sample volumes. Sample throughput 4–6 greater reported similar methods. According Blue Applicability Grade Index (BAGI) metric, considered "practical" scored 62.5. used measure samples collected from Southern Ocean. concentrations < LoD-35 LoD-48 nM, respectively. This study offers a systematic standardized MA analysis can significantly advance systems.

Language: Английский

---

Observation of the Water–HNSO₂ Complex

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(8), P. 5455 - 5460

Published: Feb. 15, 2024

Sulfamic acid (NH2SO3H, SFA) is supposed to play an important role in aerosol new particle formation (NPF) the atmosphere, and its mainly arises from SO3–NH3 reaction system which weakly bonded donor–acceptor complexes such as SO3···NH3 isomeric HNSO2···H2O have been proposed key intermediates. In this study, we reveal first spectroscopic observation of two forms a solid Ar matrix at 10 K. The major form consists intermolecular H bonds by forming six-membered ring structure with calculated dissociation energy 7.6 kcal mol–1 CCSD(T)-F12a/aug-cc-pVTZ level theory. less stable resembles SO3···H2O containing pure chalcogen bond (S···O) 7.2 mol–1. characterization matrix-isolation IR spectroscopy supported D- 18O-isotope labeling quantum chemical calculations.

Language: Английский

---

Anthropogenic Extremely Low Volatility Organics (ELVOCs) Govern the Growth of Molecular Clusters Over the Southern Great Plains During the Springtime

Journal of Geophysical Research Atmospheres, Journal Year: 2024, Volume and Issue: 129(21)

Published: Oct. 29, 2024

Abstract New particle formation (NPF) often drives cloud condensation nuclei concentrations and the processes governing nucleation of molecular clusters vary substantially in different regions. The growth these from ∼2 to >10 nm diameters is driven by availability extremely low volatility organic vapors (ELVOCs). Although pathways ELVOC oxidation biogenic terpenes are better understood, mechanistic for anthropogenic organics less well understood. We integrate measurements detailed regional model simulations understand NPF secondary aerosol at Southern Great Plain (SGP) observatory Oklahoma compare with a site within Bankhead National Forest (BNF) Alabama, southeast USA. During our two simulated event days, rates predicted be least an order magnitude higher SGP compared BNF largely due lower sulfuric acid (H 2 SO 4 ) BNF. Among mechanisms WRF‐Chem, we find that dimethylamine (DMA) + H mechanism dominates SGP. ELVOCs critical explaining particles observed Treating as semisolid, strong diffusion limitations vapor uptake phase, brings predictions into closer agreement observations. also simulate non‐NPF days show low‐level clouds reduce photochemical activity corresponding reductions concentrations, thereby lack NPF.

Language: Английский

---