Iodine oxoacids enhance nucleation of sulfuric acid particles in the atmosphere

Science, Journal Year: 2023, Volume and Issue: 382(6676), P. 1308 - 1314

Published: Dec. 14, 2023

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

Language: Английский

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Significant contributions of trimethylamine to sulfuric acid nucleation in polluted environments

npj Climate and Atmospheric Science, Journal Year: 2023, Volume and Issue: 6(1)

Published: June 27, 2023

Abstract As one of the least understood aerosol processes, nucleation can be a dominant source atmospheric aerosols. Sulfuric acid (SA)-amine binary with dimethylamine (DMA) has been recognized as governing mechanism in polluted continental boundary layer. Here we demonstrate importance trimethylamine (TMA) for complex atmosphere and propose molecular-level SA-DMA-TMA ternary an improvement upon conventional mechanism. Using proposed mechanism, could connect gaseous amines to SA-amine cluster signals measured urban Beijing. Results show that TMA accelerate SA-DMA-based new particle formation Beijing by 50–100%. Considering global abundance DMA, our findings imply comparable DMA layer, probably higher contributions from rural environments future controlled emissions.

Language: Английский

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Enhancement of Atmospheric Nucleation Precursors on Iodic Acid-Induced Nucleation: Predictive Model and Mechanism

Environmental Science & Technology, Journal Year: 2023, Volume and Issue: 57(17), P. 6944 - 6954

Published: April 21, 2023

Iodic acid (IA) has recently been recognized as a key driver for new particle formation (NPF) in marine atmospheres. However, the knowledge of which atmospheric vapors can enhance IA-induced NPF remains limited. The unique halogen bond (XB)-forming capacity IA makes it difficult to evaluate enhancing potential (EP) target compounds on based widely studied sulfuric systems. Herein, we employed three-step procedure EP nucleation precursors NPF. First, evaluated 63 by simulating free energies (ΔG) IA-containing dimer clusters. Among all clusters, 44 contained XBs, demonstrating that XBs are frequently formed. Based calculated ΔG values, quantitative structure–activity relationship model was developed evaluating other precursors. Second, amines and O/S-atom-containing acids were found have high EP, with diethylamine (DEA) yielding highest combining both concentration considered Finally, studying larger (IA)1–3(DEA)1–3 IA-DEA system merely 0.1 ppt (2.5×106 cm–3) DEA yields comparable rates IA–iodous system.

Language: Английский

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Atmospheric new particle formation from the CERN CLOUD experiment

Nature Geoscience, Journal Year: 2023, Volume and Issue: 16(11), P. 948 - 957

Published: Nov. 1, 2023

Language: Английский

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Low‐Volatility Vapors and New Particle Formation Over the Southern Ocean During the Antarctic Circumnavigation Expedition

Journal of Geophysical Research Atmospheres, Journal Year: 2021, Volume and Issue: 126(22)

Published: Oct. 16, 2021

Abstract During summer, the Southern Ocean is largely unaffected by anthropogenic emissions, which makes this region an ideal place to investigate marine natural aerosol sources and processes. A better understanding of key constrain preindustrial state reduce radiative forcing uncertainty in global climate models. We report concentrations gaseous sulfuric acid, iodic methanesulfonic acid (MSA) together with a characterization new particle formation (NPF) events over large stretch Ocean. Measurements were conducted on board Russian icebreaker Akademik Tryoshnikov from January March 2017. Iodic characterized particular diurnal cycle reduced concentration around noon, suggesting lower yield when solar irradiance higher. Gaseous MSA does not have measured gas condensed phase are compatible species being primarily produced via heterogeneous oxidation dimethyl sulfide subsequent partitioning into phase. also found that NPF boundary layer mainly driven but it occurred very rarely vast geographical area probed did contribute cloud condensation nuclei budget directly observable manner. Despite near absence layer, Aitken mode particles frequently measured, supporting hypothesis free tropospheric source. participate nucleation, however, may growth aqueous

Language: Английский

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DMS emissions from the Arctic marginal ice zone

Elementa Science of the Anthropocene, Journal Year: 2021, Volume and Issue: 9(1)

Published: Jan. 1, 2021

Phytoplankton blooms in the Arctic marginal ice zone (MIZ) can be prolific dimethylsulfide (DMS) producers, thereby influencing regional aerosol formation and cloud radiative forcing. Here we describe distribution of DMS its precursor dimethylsulfoniopropionate (DMSP) across Baffin Bay receding edge early summer 2016. Overall, total DMSP (DMSPt) increased towards warmer waters Atlantic origin concurrently with more advanced ice-melt bloom stages. Relatively high DMSPt (medians 6.3 70 nM, respectively) were observed surface layer (0–9 m depth), very values (reaching 74 524 at subsurface biomass maximum (15–30 depth). Microscopic pigment analyses indicated that peaks associated Phaeocystis pouchetii, which bloomed Atlantic-influenced reached unprecedented levels Bay. In waters, concentrations DMS:DMSPt ratios higher MIZ 12 nM 0.15, than fully ice-covered or ice-free conditions, potentially enhanced phytoplanktonic release bacterial cleavage (high dddP:dmdA gene ratios). Mean sea–air fluxes (µmol m–2 d–1) from 0.3 to 10 open (maximum 26) owing concurrent trends near-surface physical drivers gas exchange. Using remotely sensed sea-ice coverage a compilation flux data, estimated pan-Arctic emission (EDMS, MIZ) was 5–13 Gg S yr–1. North 80°N, EDMS, might have by around ± 4% yr–1 between 2003 2014, likely exceeding open-water emissions June July. We conclude must taken into account evaluate plankton-climate feedbacks Arctic.

Language: Английский

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Understanding Sources and Drivers of Size-Resolved Aerosol in the High Arctic Islands of Svalbard Using a Receptor Model Coupled with Machine Learning

Environmental Science & Technology, Journal Year: 2022, Volume and Issue: 56(16), P. 11189 - 11198

Published: July 25, 2022

Atmospheric aerosols are important drivers of Arctic climate change through aerosol–cloud–climate interactions. However, large uncertainties remain on the sources and processes controlling particle numbers in both fine coarse modes. Here, we applied a receptor model an explainable machine learning technique to understand from 10 nm 20 μm Svalbard. Nucleation, biogenic, secondary, anthropogenic, mineral dust, sea salt blowing snow their major environmental were identified. Our results show that monthly variations particles highly size/source dependent regulated by meteorology. Secondary nucleation largest contributors potential cloud condensation nuclei (CCN, number with diameter larger than 40 as proxy) Arctic. Nonlinear responses temperature found for local dust CCN, highlighting importance melting ice snow. These indicate aerosol factors will respond rapid warming differently nonlinear fashion.

Language: Английский

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Sea Ice Microbiota in the Antarctic Peninsula Modulates Cloud-Relevant Sea Spray Aerosol Production

Frontiers in Marine Science, Journal Year: 2022, Volume and Issue: 9

Published: June 16, 2022

Sea spray aerosol (SSA) formation plays a major role in the climate system. The Antarctic Peninsula (AP) is affected by greatest warming occurring Southern Ocean; changes cryospheric and biological processes are being observed. Whilst there some evidence that organic material produced ice algae and/or phytoplankton high Arctic contributes to SSA, less known about (sympagic) regions. To gain insight into influence of biology biogeochemistry on atmospheric aerosol, we report simultaneous water-air measurements made means situ chamber experiments. For first time, present methodology showing controlled plunging jet settings do not cause cell disruption studied sea ecosystems. Larger cells (>20 µm; mainly diatoms) tend sediment at bottom (during 24h experiment) likely have minor SSA production. When comparing four experiments - find two producing more ones with highest abundance nanophytoplankton (<20 nanoflagellates) as well viruses. Our marine biogeochemical data show broad groups dissolved carbon: one rich carbohydrates proteic humic-like substances; latter enhancing This work provides unique insights productivity modulates production, potentially significant impacts. Further studies these types advised order see how microbiology impacts cycling elements aerosols formed processed cold

Language: Английский

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Analysis of reduced and oxidized nitrogen-containing organic compounds at a coastal site in summer and winter

Atmospheric chemistry and physics, Journal Year: 2022, Volume and Issue: 22(5), P. 3045 - 3065

Published: March 8, 2022

Abstract. Nitrogen-containing organic compounds, which may be directly emitted into the atmosphere or form via reactions with prevalent reactive nitrogen species (e.g., NH3, NOx, NO3), have important but uncertain effects on climate and human health. Using gas liquid chromatography soft ionization high-resolution mass spectrometry, we performed a molecular-level speciation of functionalized compounds at coastal site Long Island Sound in summer (during 2018 Tropospheric Ozone Study – LISTOS campaign) winter. This region often experiences poor air quality due to emissions anthropogenic, biogenic, marine-derived their chemical transformation products. We observed range containing oxygen, nitrogen, and/or sulfur atoms resulting from these direct transformations, including photochemical aqueous-phase processing that was more pronounced winter, respectively. In both nitrogen-containing aerosols dominated distribution particle-phase ionized by our analytical techniques, 85 % 68 total measured ion abundance atom, particles included reduced functional groups amines, imines, azoles) common NOz contributors organonitrates). Reduced particle phase were frequently paired oxygen-containing elsewhere molecule, prevalence rivaled oxidized detected methods. Supplemental gas-phase measurements, collected adsorptive samplers analyzed novel chromatography-based method, suggest are possible contributing precursors particles. Altogether, this work highlights less-studied northeastern US potentially other regions similar marine source signatures.

Language: Английский

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Frequent new particle formation at remote sites in the subboreal forest of North America

Atmospheric chemistry and physics, Journal Year: 2022, Volume and Issue: 22(4), P. 2487 - 2505

Published: Feb. 24, 2022

Abstract. The frequency and intensity of new particle formation (NPF) over remote forest regions in the temperate boreal zones, thus importance NPF for aerosol budget life cycle pristine atmosphere, remains controversial. Whereas has been shown to occur relatively frequently at several sites Scandinavia, it was found be nearly absent a mid-continental site Siberia. To explore this issue further, we made measurements size distributions between 10 420 nm diameter two transition region British Columbia, Canada. covered 23 d during month June 2019, time when typically reaches its seasonal maximum midlatitude regions. These are first such near-pristine on North American continent. Although were only 150 km apart, there clear differences them. At Eagle Lake site, occurred daily, nucleation-mode concentrations reached above 5000 cm−3. In contrast, Nazko River six events 11 d, about 800 reasons difference could not conclusively resolved with available data; they may include air mass origins, preexisting aerosols, density type cover surrounding contrast observations other environments, that our nighttime just as daytime. Together lack identifiable sources sulfuric acid precursor species fetch sites, suggests nucleation extremely low volatility organics predominant mechanism. Our results indicate extended measurement campaigns more comprehensive set instrumentation investigate role America essential deeper scientific understanding important process global budget.

Language: Английский

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