Science Advances, Journal Year: 2020, Volume and Issue: 6(22)
Published: May 27, 2020
NO x is important for particle growth as it can participate in HOM formation and alter the volatility distribution.
Language: Английский
Journal of Geophysical Research Atmospheres, Journal Year: 2019, Volume and Issue: 124(13), P. 7098 - 7146
Published: June 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.
Language: Английский
Citations
366
Geophysical Research Letters, Journal Year: 2020, Volume and Issue: 48(4)
Published: Dec. 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
Language: Английский
Citations
241
Nature Communications, Journal Year: 2019, Volume and Issue: 10(1)
Published: Sept. 25, 2019
Abstract Over Boreal regions, monoterpenes emitted from the forest are main precursors for secondary organic aerosol (SOA) formation and primary driver of growth new particles to climatically important cloud condensation nuclei (CCN). Autoxidation leads rapid Highly Oxygenated Molecules (HOM). We have developed first model with near-explicit representation atmospheric particle (NPF) HOM formation. The can reproduce observed NPF, gas-phase composition SOA over forest. During spring, increases CCN concentration by ~10 % causes a direct radiative forcing −0.10 W/m 2 . In contrast, NPF reduces number at updraft velocities < 0.2 m/s, +0.15 Hence, while contributes climate cooling, result in warming
Language: Английский
Citations
181
Science Advances, Journal Year: 2020, Volume and Issue: 6(6)
Published: Feb. 6, 2020
Tracking reactive organic carbon in the atmosphere is critical to advancing our understanding of air quality and climate.
Language: Английский
Citations
171
Science Advances, Journal Year: 2020, Volume and Issue: 6(11)
Published: March 13, 2020
Highly oxygenated organic molecules (HOMs) are formed from the oxidation of biogenic and anthropogenic gases affect Earth's climate air quality by their key role in particle formation growth. While these gas phase has been extensively studied, complexity aerosol (OA) lack suitable measurement techniques have hindered investigation fate post-condensation, although further reactions proposed. We report here novel real-time measurements species phase, achieved using our recently developed extractive electrospray ionization time-of-flight mass spectrometer (EESI-TOF). Our results reveal that condensed-phase rapidly alter OA composition contribution HOMs to mass. In consequence, atmospheric cannot be described solely terms volatility, but particle-phase must considered describe HOM effects on overall life cycle global carbon budget.
Language: Английский
Citations
169
Journal of Aerosol Science, Journal Year: 2020, Volume and Issue: 149, P. 105621 - 105621
Published: July 3, 2020
Language: Английский
Citations
167
Atmospheric chemistry and physics, Journal Year: 2020, Volume and Issue: 20(2), P. 1183 - 1199
Published: Jan. 31, 2020
Abstract. Gas-phase autoxidation of organics can generate highly oxygenated organic molecules (HOMs) and thus increase secondary aerosol production enable new-particle formation. Here we present a new implementation the volatility basis set (VBS) that explicitly resolves peroxy radical (RO2) products formed via autoxidation. The model includes strong temperature dependence for as well explicit termination RO2, including reactions with NO, HO2, other RO2. RO2 cross-reactions produce dimers (ROOR). We explore NOx this chemistry, showing strongly influences intrinsic distribution NO suppress under conditions typically found in atmosphere.
Language: Английский
Citations
165
Atmospheric chemistry and physics, Journal Year: 2020, Volume and Issue: 20(1), P. 515 - 537
Published: Jan. 15, 2020
Abstract. Recent studies have recognised highly oxygenated organic molecules (HOMs) in the atmosphere as important formation of secondary aerosol (SOA). A large number focused on HOM from oxidation biogenically emitted monoterpenes. However, anthropogenic vapours has so far received much less attention. Previous identified importance aromatic volatile compounds (VOCs) for SOA formation. In this study, we investigated several compounds, benzene (C6H6), toluene (C7H8), and naphthalene (C10H8), their potential to form HOMs upon reaction with hydroxyl radicals (OH). We performed flow tube experiments all three VOCs detail Jülich Plant Atmosphere Chamber (JPAC). JPAC, also response NOx seed aerosol. Using a nitrate-based chemical ionisation mass spectrometer (CI-APi-TOF), observed reactor first OH attack. naphthalene, which were injected at lower concentrations, multi-generation seemed impact composition. tested more system allowed studying longer residence times. The results showed that apparent molar yield under our experimental conditions varied 4.1 % 14.0 %, strong dependence concentration, indicating majority formed through multiple OH-oxidation steps. composition spectrum supported hypothesis. By injecting only phenol into chamber, found cannot be solely responsible experiments. When was added changed many nitrogen-containing products CI-APi-TOF. Upon injection, loss rate higher than predicted by irreversible condensation, suggesting some undetected intermediates condensed onto aerosol, is line hypothesis oxidation. Based results, conclude systems strongly depend VOC concentration are needed fully understand effect and, consequently, SOA. suggest chamber may explain part variability yields reported literature advise monitoring future studies.
Language: Английский
Citations
162
Nature Geoscience, Journal Year: 2022, Volume and Issue: 15(4), P. 255 - 261
Published: April 1, 2022
Language: Английский
Citations
154
Geophysical Research Letters, Journal Year: 2021, Volume and Issue: 48(7)
Published: March 22, 2021
Abstract Intense and frequent new particle formation (NPF) events have been observed in polluted urban environments, yet the dominant mechanisms are still under debate. To understand key species governing processes of NPF we conducted comprehensive measurements downtown Beijing during January–March, 2018. We performed detailed analyses on sulfuric acid cluster composition budget, as well chemical physical properties oxidized organic molecules (OOMs). Our results demonstrate that fast clustering (H 2 SO 4 ) base triggered events, OOMs further helped grow newly formed particles toward climate‐ health‐relevant sizes. This synergistic role H , species, is likely representative environments where abundant usually co‐exist, with moderately low volatility when produced high NO x concentrations.
Language: Английский
Citations
150