Global Distribution of the Phase State and Mixing Times within Secondary Organic Aerosol Particles in the Troposphere Based on Room-Temperature Viscosity Measurements

Maclean, Adrian M.; Liu, Ying; Crescenzo, Giuseppe V.; Smith, Natalie R.; Karydis, Vlassis A.; Tsimpidi, Alexandra P.; Butenhoff, C. L.; Faiola, Celia; Lelieveld, Jos; Nizkorodov, Sergey A.; Shiraiwa, Manabu; Bertram, Allan K.

doi:10.1021/acsearthspacechem.1c00296

Cited by 27 publications

(34 citation statements)

References 131 publications

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“…There is some relationship with temperature in dOAER/dt, and higher temperatures are more supportive of continued evaporation as the plume ages, while lower temperatures tend toward no net change or net condensation. This temperature correlation may be related to the effect of temperature on OA volatility as well as OA particle-phase diffusivity/viscosity (Maclean et al, 2021). The positive slopes seen at lower concentrations combined with the first transect being at least 30 min downwind (Fig.…”

Section: Observationsmentioning

confidence: 91%

Aerosol size distribution changes in FIREX-AQ biomass burning plumes: the impact of plume concentration on coagulation and OA condensation/evaporation

et al. 2022

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Abstract. The evolution of organic aerosol (OA) and aerosol size distributions within smoke plumes is uncertain due to the variability in rates of coagulation and OA condensation/evaporation between different smoke plumes and at different locations within a single plume. We use aircraft data from the FIREX-AQ campaign to evaluate differences in evolving aerosol size distributions, OA, and oxygen to carbon ratios (O:C) between and within smoke plumes during the first several hours of aging as a function of smoke concentration. The observations show that the median particle diameter increases faster in smoke of a higher initial OA concentration (>1000 µg m−3), with diameter growth of over 100 nm in 8 h – despite generally having a net decrease in OA enhancement ratios – than smoke of a lower initial OA concentration (<100 µg m−3), which had net increases in OA. Observations of OA and O:C suggest that evaporation and/or secondary OA formation was greater in less concentrated smoke prior to the first measurement (5–57 min after emission). We simulate the size changes due to coagulation and dilution and adjust for OA condensation/evaporation based on the observed changes in OA. We found that coagulation explains the majority of the diameter growth, with OA evaporation/condensation having a relatively minor impact. We found that mixing between the core and edges of the plume generally occurred on timescales of hours, slow enough to maintain differences in aging between core and edge but too fast to ignore the role of mixing for most of our cases.

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Section: Observationsmentioning

confidence: 91%

Aerosol size distribution changes in FIREX-AQ biomass burning plumes: the impact of plume concentration on coagulation and OA condensation/evaporation

et al. 2022

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“…The state-of-the-art is at the single particle level, which can be probed using various approaches ranging from cavity ring-down spectroscopy of levitated particles to cryogenic transmission electron microscopy of submicrometer particles under dynamic conditions . Parametrizations of the aerosol phase state have supported numerical simulations for environments across the U.S., which show that high-viscosity particles are likely common in drier areas (e.g., in the West) and at high altitudes. , …”

Section: Phase Transitionsmentioning

confidence: 99%

“…12 Parametrizations of the aerosol phase state have supported numerical simulations for environments across the U.S., which show that high-viscosity particles are likely common in drier areas (e.g., in the West) 13 and at high altitudes. 13,14 ■…”

Section: ■ Phase Transitionsmentioning

confidence: 99%

Virtual Issue on Atmospheric Aerosol Research

2022

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Metrics & MoreArticle Recommendations F ollowing our successful 2020 Virtual Issue on Atmospheric Chemistry Research, 1 we now present a second Virtual Issue on the topic, with a specific emphasis on papers focusing on atmospheric aerosols (particulate matter) that recently appeared in The Journal of Physical Chemistry A and in ACS Earth and Space Chemistry. The purposes of this Virtual Issue are to highlight the various topics and scientific themes of interest to the two journals, to showcase some of the new and exciting insights that have been made during two particularly hard years for science and engineering, to provide an entry point for scientists who are considering entering the field, and to offer starting material for a possible upper-level undergraduate or graduate course on the topic of atmospheric aerosols.

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“…CC BY 4.0 License. Maclean et al, 2021). According to the new parameterization method introduced by Li et al (2020b), Tg of OA (Tg,org) at dry conditions was estimated based on OA volatility distribution and the ratio of oxygen to carbon (O:C, "Aiken-Ambient" method).…”

Section: Predictions Of Glass Transition Temperature and Viscosity Of...mentioning

confidence: 99%

Aging impact on sources, volatility, and viscosity of organic aerosols in the Chinese outflows

Feng

Wang

et al. 2022

Preprint

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Abstract. To investigate the aging impact on sources, volatility, and viscosity of organic aerosols (OA) in the Chinese outflows, a high-resolution time-of-flight aerosol mass spectrometer (HR-AMS) coupled with a thermodenuder (TD) was deployed in the spring of 2018 in Dongying, which is a regional receptor site of metropolitan emissions in North China Plain (NCP). The average mass concentration of PM1 was 31.5 ± 22.7 μg m–3, which was mainly composed of nitrate (33 %) and OA (25 %). The source apportionment results show the OA was mainly contributed by oxygenated OA (OOA) from secondary sources, including background-OOA (33 %) representing a background concentration of OA (2.6 μg m–3) in the NCP area, and transported-OOA (33 %) oxidizing from urban emissions. The other two factors include aged hydrocarbon-liked OA (aged-HOA, 28 %) from transported vehicle emissions and biomass burning OA (BBOA, 5 %) from local open burnings. The volatility of total OA (average C* = 3.2×10–4 µg m–3) in this study is generally lower than those in previous field studies, which is mainly due to the high OA oxidation level resulting from aging processes during transport. The volatilities of OA factors follow the order of background-OOA (average C* = 2.7×10–5 μg m–3) < transported-OOA (3.7×10–4 μg m–3) < aged-HOA (8.1×10–4 μg m–3) < BBOA (0.012 μg m–3), indicating the probable existence of oligomers. The viscosity estimation suggests that the majority of ambient OA in this study behaves as semi-solid (60 %), liquifies at higher RH (21 %), and solidifies (19 %) during noon time when the RH is low and the oxidation level is high. Finally, the estimated mixing time of OA varies dramatically from minutes at night to years in the afternoon, emphasizing the necessity to consider its dynamic kinetic limits when modeling OA. In general, the overall results of this study improve the understanding of the aging impact on OA volatility and viscosity.

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Global Distribution of the Phase State and Mixing Times within Secondary Organic Aerosol Particles in the Troposphere Based on Room-Temperature Viscosity Measurements

Cited by 27 publications

References 131 publications

Aerosol size distribution changes in FIREX-AQ biomass burning plumes: the impact of plume concentration on coagulation and OA condensation/evaporation

Aerosol size distribution changes in FIREX-AQ biomass burning plumes: the impact of plume concentration on coagulation and OA condensation/evaporation

Virtual Issue on Atmospheric Aerosol Research

Aging impact on sources, volatility, and viscosity of organic aerosols in the Chinese outflows

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