Pan-Arctic seasonal cycles and long-term trends of aerosol properties from 10 observatories

Atmospheric chemistry and physics, Journal Year: 2022, Volume and Issue: 22(5), P. 3067 - 3096

Published: March 8, 2022

Abstract. Even though the Arctic is remote, aerosol properties observed there are strongly influenced by anthropogenic emissions from outside Arctic. This particularly true for so-called haze season (January through April). In summer (June September), when atmospheric transport patterns change, and precipitation more frequent, local sources, i.e., natural sources of aerosols precursors, play an important role. Over last few decades, significant reductions in have taken place. At same time a large body literature shows evidence that undergoing fundamental environmental changes due to climate forcing, leading enhanced processes may impact properties. this study, we analyze 9 chemical species 4 particle optical 10 observatories (Alert, Kevo, Pallas, Summit, Thule, Tiksi, Barrow/Utqiaġvik, Villum, Gruvebadet Zeppelin Observatory – both at Ny-Ålesund Research Station) understand contributions. Variables include equivalent black carbon, particulate sulfate, nitrate, ammonium, methanesulfonic acid, sodium, iron, calcium potassium, as well scattering absorption coefficients, single albedo Ångström exponent. First, annual cycles investigated, which despite emission still show phenomenon. Second, long-term trends studied using Mann–Kendall Theil–Sen slope method. We find total 41 over full station records, spanning than decade, compared 26 decadal trends. The majority significantly declining tracers occurred during period, driven between 1990 2000. For no uniform picture has emerged. Twenty-six percent trends, 19 out 73, significant, those 5 positive 14 negative. Negative not only such carbon but also indicators acid non-sea-salt Alert. Positive sulfate Gruvebadet. No clear change contribution can be yet. However, testing sensitivity method, monotonic around % yr−1 property needed detect trend within one decade. highlights efforts beyond decade capture smaller changes. It ongoing Arctic, where interannual variability high, with forest fire their influence on population. To investigate climate-change-induced population resulting feedback, observations specific needed, microphysical size distributions, used identify populations captured mass-oriented methods bulk composition.

Language: Английский

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Progress in Unraveling Atmospheric New Particle Formation and Growth Across the Arctic

Geophysical Research Letters, Journal Year: 2021, Volume and Issue: 48(14)

Published: July 3, 2021

Abstract New particle formation (NPF) and growth can be an important source of cloud condensation nuclei for the Arctic atmosphere, where is sensitive to their availability. Low‐level clouds influence energy budget, likely contribute amplified warming. Molecular information NPF rarely reported, despite its importance determine sources condensing vapors nucleation mechanisms. Beck et al. (2020, https://doi.org/10.1029/2020gl091334 ) shed light on complexity at two locations. They reveal that chemical drivers are diverse across Arctic. This advance in knowledge calls similar studies throughout all seasons various environments obtain a more systematic understanding growth.

Language: Английский

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High Gas-Phase Methanesulfonic Acid Production in the OH-Initiated Oxidation of Dimethyl Sulfide at Low Temperatures

Environmental Science & Technology, Journal Year: 2022, Volume and Issue: 56(19), P. 13931 - 13944

Published: Sept. 22, 2022

Dimethyl sulfide (DMS) influences climate via cloud condensation nuclei (CCN) formation resulting from its oxidation products (mainly methanesulfonic acid, MSA, and sulfuric H2SO4). Despite their importance, accurate prediction of MSA H2SO4 DMS remains challenging. With comprehensive experiments carried out in the Cosmics Leaving Outdoor Droplets (CLOUD) chamber at CERN, we show that decreasing temperature +25 to −10 °C enhances gas-phase production by an order magnitude OH-initiated oxidation, while is modestly affected. This leads a H2SO4-to-MSA ratio (H2SO4/MSA) smaller than one low temperatures, consistent with field observations polar regions. updated mechanism, find methanesulfinic CH3S(O)OH, MSIA, forms large amounts MSA. Overall, our results reveal yields are factor 2–10 higher those predicted widely used Master Chemical Mechanism (MCMv3.3.1), NOx effect less significant temperature. Our mechanism explains high rates observed observations, especially thus, substantiating greater importance natural sulfur cycle CCN formation. will improve interpretation present-day historical H2SO4/MSA measurements.

Language: Английский

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A central arctic extreme aerosol event triggered by a warm air-mass intrusion

Nature Communications, Journal Year: 2022, Volume and Issue: 13(1)

Published: Sept. 8, 2022

Abstract Frequency and intensity of warm moist air-mass intrusions into the Arctic have increased over past decades been related to sea ice melt. During our year-long expedition in remote central Ocean, a record-breaking increase temperature, moisture downwelling-longwave radiation was observed mid-April 2020, during an intrusion carrying air pollutants from northern Eurasia. The two-day intrusion, caused drastic changes aerosol size distribution, chemical composition particle hygroscopicity. Here we show how transformed low-particle environment area comparable central-European urban setting. Additionally, resulted explosive cloud condensation nuclei, which can direct effects on clouds’ radiation, their precipitation patterns, lifetime. Thus, unless prompt actions significantly reduce emissions source regions are taken, such events expected continue affect climate.

Language: Английский

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Physical and Chemical Properties of Cloud Droplet Residuals and Aerosol Particles During the Arctic Ocean 2018 Expedition

Journal of Geophysical Research Atmospheres, Journal Year: 2022, Volume and Issue: 127(11)

Published: May 25, 2022

Detailed knowledge of the physical and chemical properties sources particles that form clouds is especially important in pristine areas like Arctic, where particle concentrations are often low observations sparse. Here, we present situ cloud aerosol measurements from central Arctic Ocean August-September 2018 combined with air parcel source analysis. We provide direct experimental evidence Aitken mode (particles diameters ≲70 nm) significantly contribute to condensation nuclei (CCN) or droplet residuals, after freeze-up sea ice transition toward fall. These were associated spent more time over pack ice, while size distributions dominated by accumulation ≳70 showed a stronger contribution oceanic slightly different regions. This was accompanied changes average composition an increased relative organic material Addition mass due aqueous-phase chemistry during in-cloud processing probably small given fact observed very similar both whole-air residual data. aerosol-cloud interaction valuable insight into origin CCN Ocean.

Language: Английский

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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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A full year of aerosol size distribution data from the central Arctic under an extreme positive Arctic Oscillation: insights from the Multidisciplinary drifting Observatory for the Study of Arctic Climate (MOSAiC) expedition

Atmospheric chemistry and physics, Journal Year: 2023, Volume and Issue: 23(1), P. 389 - 415

Published: Jan. 11, 2023

Abstract. The Arctic environment is rapidly changing due to accelerated warming in the region. trend driving a decline sea ice extent, which thereby enhances feedback loops surface energy budget Arctic. aerosols play an important role radiative balance and hence climate response region, yet direct observations of over Ocean are limited. In this study, we investigate annual cycle aerosol particle number size distribution (PNSD), concentration (PNC), black carbon (BC) mass central during Multidisciplinary drifting Observatory for Study Climate (MOSAiC) expedition. This first continuous, year-long data set PNSD ever collected Ocean. We use k-means cluster analysis, FLEXPART simulations, inverse modeling evaluate seasonal patterns influence different source regions on population. Furthermore, compare land-based sites across Arctic, using both long-term measurements year MOSAiC expedition (2019–2020), interannual variability give context characteristics from within Our analysis identifies that, overall, exhibits typical aerosols, including anthropogenic haze winter secondary processes summer. pattern corresponds global radiation, air temperature, timing melting/freezing, drive changes transport processes. winter, Norilsk region Russia/Siberia was dominant signals BC observations, contributed higher accumulation-mode PNC concentrations than at observatories. also show that wintertime Oscillation (AO) phenomenon, reported achieve record-breaking positive phase January–March 2020, explains unusual magnitude compared longer-term observations. summer, PNCs nucleation Aitken modes enhanced; however, were notably lower pack further south. presented herein provides current snapshot characterized by rapid changes, will be crucial improving model predictions, understanding linkages between environmental processes, investigating impacts change future studies.

Language: Английский

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Phylogeny-metabolism dual-directed single-cell genomics for dissecting and mining ecosystem function by FISH-scRACS-seq

The Innovation, Journal Year: 2025, Volume and Issue: 6(3), P. 100759 - 100759

Published: Jan. 18, 2025

Microbiome-wide association studies (MWASs) have uncovered microbial markers linked to ecosystem traits, but the mechanisms underlying their functions can remain elusive. This is largely due challenges in validating situ metabolic activities and tracing such individual genomes. Here, we introduced a phylogeny-metabolism dual-directed single-cell genomics approach called fluorescence-in situ-hybridization-guided Raman-activated sorting sequencing (FISH-scRACS-seq). It directly localizes cells from target taxon via an FISH probe for marker organism, profiles Raman spectra, sorts of taxonomy metabolism, produces indexed, high-coverage, precisely-one-cell From cyclohexane-contaminated seawater, representing MWAS-derived γ-Proteobacteria that are actively degrading cyclohexane were identified Raman, respectively, then sorted sequenced one-cell full In Pseudoalteromonas fuliginea cell, discovered three-component cytochrome P450 system convert cyclohexanol vitro, previously unknown group cyclohexane-degrading enzymes organisms. Therefore, by unveiling enzymes, pathways, genomes, cellular specifically those organisms with ecological relevance at resolution, FISH-scRACS-seq rational generally applicable dissecting mining microbiota functions.

Language: Английский

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Observations of high-time-resolution and size-resolved aerosol chemical composition and microphysics in the central Arctic: implications for climate-relevant particle properties

Atmospheric chemistry and physics, Journal Year: 2025, Volume and Issue: 25(4), P. 2207 - 2241

Published: Feb. 19, 2025

Abstract. Aerosols play a critical role in the Arctic's radiative balance, influencing solar radiation and cloud formation. Limited observations central Arctic leave gaps understanding aerosol dynamics year-round, affecting model predictions of climate-relevant properties. Here, we present first annual high-time-resolution submicron chemical composition during Ocean 2018 (AO2018) 2019–2020 Multidisciplinary drifting Observatory for Study Climate (MOSAiC) expeditions. Seasonal variations mass concentrations were found to be driven by typical seasonal regimes resemble those pan-Arctic land-based stations. Organic aerosols dominated pristine summer, while anthropogenic sulfate prevailed autumn spring under haze conditions. Ammonium, which impacts acidity, was consistently less abundant, relative sulfate, compared lower latitudes Arctic. Cyclonic (storm) activity have significant influence on variability enhancing emissions from local sources transport remote aerosol. Local wind-generated particles contributed up 80 % (20 %) condensation nuclei population (spring). While analysis presented herein provides current baseline, will serve improve climate region, it also underscores importance integrating short-timescale processes, such as wind-driven blowing snow open leads/ocean simulations. This is particularly important, given decline mid-latitude increase ones.

Language: Английский

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Formation of condensable organic vapors from anthropogenic and biogenic volatile organic compounds (VOCs) is strongly perturbed by NO<sub><i>x</i></sub> in eastern China

Atmospheric chemistry and physics, Journal Year: 2021, Volume and Issue: 21(19), P. 14789 - 14814

Published: Oct. 6, 2021

Abstract. Oxygenated organic molecules (OOMs) are the crucial intermediates linking volatile compounds (VOCs) to secondary aerosols (SOAs) in atmosphere, but comprehensive understanding of characteristics OOMs and their formation from VOCs is still missing. Ambient observations using recently developed mass spectrometry techniques limited, especially polluted urban atmospheres where oxidants extremely variable complex. Here, we investigate OOMs, measured by a nitrate-ion-based chemical ionization spectrometer at Nanjing eastern China, through performing positive matrix factorization on binned spectra (binPMF). The binPMF analysis reveals three factors about anthropogenic VOC (AVOC) daytime chemistry, isoprene-related factors, biogenic (BVOC) nighttime nitrated phenols. All influenced NOx different ways extents. Over 1000 non-nitro have been identified then reconstructed selected solution binPMF, 72 % total signals contributed nitrogen-containing mostly regarded as nitrates formed peroxy radicals terminated nitric oxide or nitrate-radical-initiated oxidations. Moreover, multi-nitrates account for 24 signals, indicating significant presence multiple generations, isoprene (e.g., C5H10O8N2 C5H9O10N3). Additionally, distribution OOM concentration carbon number confirms precursors driven AVOCs mixed with enhanced BVOCs during summer. Our results highlight decisive role densely populated areas, encourage more studies dramatic interactions between emissions.

Language: Английский

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