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

---

Measurement report: Insights into the chemical composition and origin of molecular clusters and potential precursor molecules present in the free troposphere over the southern Indian Ocean: observations from the Maïdo Observatory (2150 m a.s.l., Réunion)

Atmospheric chemistry and physics, Journal Year: 2024, Volume and Issue: 24(6), P. 3785 - 3812

Published: March 27, 2024

Abstract. New particle formation (NPF) in the free troposphere (FT) is thought to be a significant source of particles over oceans. The entrainment initially formed marine FT further suspected major contributor cloud condensation nuclei (CCN) number concentrations boundary layer (BL). Yet, little known about process and, more broadly, composition FT, which remains poorly explored due access difficulties. Here we report measurements performed April 2018 at Maïdo Observatory with nitrate-based chemical ionization atmospheric pressure interface time-of-flight mass spectrometer, have allowed first molecular-level characterization remote composition. A molecules and clusters were identified classified into nine groups according their composition; among species, containing methanesulfonic acid (MSA) C2 amines show signals that are on average significantly higher when site under conditions representative (compared BL). correlation analysis revealed apparent connections between compounds several variables concurrently measured (under conditions) or related air history, suggesting oxalic acid, malonic observed could terrestrial origin, with, addition, possible for amines, while iodic sulfur maleic dominant origin. Identification was based standard deviation wind direction; this parameter, can easily derived from continuous site, shown part study relevant tracer compared predictions Meso-NH model. Similar other high-altitude sites, mainly encountered night Maïdo; therefore, link NPF not established, research needed assess precursors nanoparticle FT.

Language: Английский

---

Chemical precursors of new particle formation in coastal New Zealand

Atmospheric chemistry and physics, Journal Year: 2023, Volume and Issue: 23(7), P. 3955 - 3983

Published: April 4, 2023

Abstract. To reduce uncertainties in climate predictions, we need to better understand aerosol formation different environments. An important part of this is studying which chemical species are responsible for particle formation. While many advances have been made field, measurements especially lacking from marine Here, measured the composition ambient anions over 7 months at Baring Head station, located coastal New Zealand. This adds our previous work reported size distribution and investigated new environmental conditions favouring station. By combining information on ion with work, were able study precursors Our results showed that while land likely driven by sulfuric acid organic species, clean air iodine oxoacids sulfur drivers processes. These data also used characterise diurnal seasonal cycles most anion groups their geographical source regions. Bisulfate displayed a clear daytime maximum where as had morning evening maximums. Highly oxygenated molecules, other hand, abundant during night when was land-influenced. set highly valuable provide driving remote Southern Hemisphere site.

Language: Английский

---

Do bromine and surface-active substances influence the coastal atmospheric particle growth?

Heliyon, Journal Year: 2024, Volume and Issue: 10(11), P. e31632 - e31632

Published: May 21, 2024

New particle formation (NPF) is considered a major source of aerosol particles and cloud condensation nuclei (CCN); however, our understanding NPF the subsequent growth mechanisms in coastal areas remains limited. This study provides evidence frequent events followed by middle Adriatic Sea during summer months at station Rogoznica Croatia. To knowledge, this first to report such region. Our research aims improve investigating through detailed physicochemical characterization event classification. We used combination online measurements offline collection, thorough chemical analysis. results suggest role bromine process provide for its involvement with organic compounds. In addition, we demonstrated significant influence surface-active substances (SAS) on growth. have been observed air masses originating from Sea, which can serve as an important volatile compounds (VOC). shows intricate interplay between bromine, carbon (OC), SAS atmospheric growth, contributing better processes. context, also introduced new approach using semi-empirical 1st derivative method determine rate each time point that not sensitive nonlinear behavior over time. days, OC concentration measured ultrafine mode fraction was higher compared non-event days. Moreover, contrast were detected nearly all Regarding sulfuric acid, sulfate both days showed no differences. suggests acid may be primary factor influencing appearance region Rogoznica.

Language: Английский

---

Atmospheric Particle Number Concentrations and New Particle Formation over the Southern Ocean and Antarctica: A Critical Review

Atmosphere, Journal Year: 2023, Volume and Issue: 14(2), P. 402 - 402

Published: Feb. 19, 2023

The Southern Ocean (SO) and Antarctica play important roles in the global climate. new particle formation (NPF) alters availability of cloud condensation nuclei (CCN), leading to impacts on reflectance radiative budget. In this review, we introduce common instruments for measuring number concentration (PNC) size distribution (PNSD). Based observations over Antarctic some research stations, explored spatial temporal characteristics PNCs PNSDs. From SO interior Antarctic, total show a decreasing trend, present an obvious seasonal cycle, with low winter (June–August) high summer (December–February). By summarizing progress Antarctica, discuss possible precursors NPF: sulfuric acid (H2SO4, SA), methanesulfonic (CH3S(O)2OH, MSA), dimethyl sulfide ((CH3)2S, DMS), iodic (HIO3, IA), iodous (HIO2), ammonia (NH3), dimethylamine ((CH3)2NH, DMA), highly oxygenated organic molecules (HOMs) other organics vapor pressure. We also explore several nucleation mechanisms: ion-induced H2SO4 NH3, H2SO4-amines, H2SO4-DMA-H2O, H2SO4-MSA-DMA, IA-MSA, IA-DMA, heterogeneous IA-organics mechanisms environmental conditions required NPF. NPF is one main sources CCN remote marine boundary layer, such as Antarctica. Thus, contribution indirect Through could better understand PNC their

Language: Английский

---

Spatio-Temporal Distributions of the Natural Non-Sea-Salt Aerosol Over the Southern Ocean and Coastal Antarctica and Its Potential Source Regions

Tellus B, Journal Year: 2023, Volume and Issue: 75(1), P. 47 - 64

Published: Jan. 1, 2023

More than 40 years of aerosol data including concentrations particle number and nine major ions collected over the Southern Ocean coastal stations have been aggregated filtered with back trajectories to reduce risk influence from adjacent continents. That provided a rich dataset latitudinal distribution seasonality physical chemical parameters that allow insights into sources Ocean. These together statistics trajectory paths high (75% percentile) low (25% studied were used identify potential source regions respective compounds. For concentrations, MSA, non-sea-salt fractions Ca potassium most prominent found in DMS-areas close Antarctica, whereas NH4 fraction Mg located part further north geographical differences would reflect marine biota.

Language: Английский

---

Segregation of Fast-Reactive Species in Atmospheric Turbulent Flow

Published: May 12, 2023

Atmospheric turbulence, which produces chaotic motions in the planetary boundary layer, can inhibit mixing between fast-reacting species produced or released at different locations. This segregation process modifies effective rate reactions occur these species, and are not appropriately accounted for coarse resolution models since assume complete of tracers within each gridbox. Here we present a few examples LES-based simulations applied to chemically reactive forested area with high emissions biogenic hydrocarbons, an urban rich anthropogenic emissions; maritime reduced sulfur species.

Language: Английский

---

What chemical species are responsible for new particle formation and growth in the Netherlands? A hybrid positive matrix factorization (PMF) analysis using aerosol composition (ACSM) and size (SMPS)

Atmospheric chemistry and physics, Journal Year: 2023, Volume and Issue: 23(17), P. 10015 - 10034

Published: Sept. 8, 2023

Abstract. Aerosol formation acts as a sink for gas-phase atmospheric species that controls their lifetime and environmental effects. To investigate aerosol evolution in the Netherlands, hybrid positive matrix factorization (PMF) analysis was conducted using observations from May, June, September 2021 collected rural site of Cabauw central part Netherlands. The input consists full organic mass spectrum acquired time-of-flight chemical speciation monitor (ToF-ACSM), ACSM inorganic concentrations, binned particle size distribution concentrations scanning mobility sizer (SMPS). These PMF analyses discerned four factors describe composition variations: two size-driven are related to new (NPF) growth (F4 F3), well bulk driven by composition, not (F2 F1). across these shows different compounds responsible nucleation particles. smallest-diameter factor (F4) contains ammonium sulfate organics typically peaks during daytime. Newly formed particles, represented F4, mainly correlated with wind southwesterly–westerly easterly sectors transport sulfur oxides (SOx), ammonia (NH3), precursors Cabauw. As particles grow F4 F3 factors, nitrate play an increasing role, loading diurnal cycle shifts daytime nighttime maximum. Greater availability makes secondary (SOA) more influential summertime growth, principally due volatility differences produced seasonal variation photooxidation temperature.

Language: Английский

---

Evidence of nitrate-based nighttime atmospheric nucleation driven by marine microorganisms in the South Pacific

Proceedings of the National Academy of Sciences, Journal Year: 2023, Volume and Issue: 120(48)

Published: Nov. 22, 2023

Our understanding of ocean–cloud interactions and their effect on climate lacks insight into a key pathway: do biogenic marine emissions form new particles in the open ocean atmosphere? Using measurements collected ship-borne air–sea interface tanks deployed Southwestern Pacific Ocean, we identified particle formation (NPF) during nighttime that was related to plankton community composition. We show nitrate ions are only species for which abundance could support NPF rates our semicontrolled experiments. Nitrate also prevailed natural pristine atmosphere were elevated under higher sub-10 nm concentrations. hypothesize these nucleation events fueled by complex, short-term biogeochemical cycling involving microbial loop. These findings suggest perspective with previously unidentified role origin aerosol nucleation.

Language: Английский

---

Influence of open ocean biogeochemistry on aerosol and clouds: Recent findings and perspectives

Elementa Science of the Anthropocene, Journal Year: 2024, Volume and Issue: 12(1)

Published: Jan. 1, 2024

Aerosols and clouds are key components of the marine atmosphere, impacting Earth’s radiative budget with a net cooling effect over industrial era that counterbalances greenhouse gas warming, yet an uncertain amplitude. Here we report recent advances in our understanding how open ocean aerosol sources modulated by biogeochemistry they, turn, shape cloud coverage properties. We organize these findings successive steps from biogeochemical processes to particle formation nucleation sea spray emissions, further growth condensation gases, potential act as nuclei or ice nucleating particles, finally, their effects on formation, optical properties, life cycle. discuss may be impacted warming climate for biogeochemistry—climate feedbacks through aerosols clouds.

Language: Английский

---