Cloud droplet activation through oxidation of organic aerosol influenced by temperature and particle phase state

Slade, John; Shiraiwa, Manabu; Arangio, Andrea M.; Su, Hang; Pöschl, Ulrich; Wang, Jian; Knopf, Daniel A.

doi:10.1002/2016gl072424

Cited by 61 publications

(88 citation statements)

References 47 publications

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“…Despite the integral role of SOA in atmospheric processes, there remains a limited understanding of the chemical and physical changes induced in SOA as it is formed and subsequently aged. Understanding the physical state of SOA is especially important, as it can provide insight into SOA formation [12,13] and growth [14], gas-particle partitioning [15], reactive uptake on particle surfaces [16,17], and atmospheric impacts [18][19][20].…”

Section: Introductionmentioning

confidence: 99%

The Influence of Absolute Mass Loading of Secondary Organic Aerosols on Their Phase State

2018

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Absolute secondary organic aerosol (SOA) mass loading (C SOA ) is a key parameter in determining partitioning of semi-and intermediate volatility compounds to the particle phase. Its impact on the phase state of SOA, however, has remained largely unexplored. In this study, systematic laboratory chamber measurements were performed to elucidate the influence of C SOA , ranging from 0.2 to 160 µg m −3 , on the phase state of SOA formed by ozonolysis of various precursors, including α-pinene, limonene, cis-3-hexenyl acetate (CHA) and cis-3-hexen-1-ol (HXL). A previously established method to estimate SOA bounce factor (BF, a surrogate for particle viscosity) was utilized to infer particle viscosity as a function of C SOA . Results show that under nominally identical conditions, the maximum BF decreases by approximately 30% at higher C SOA , suggesting a more liquid phase state. With the exception of HXL-SOA (which acted as the negative control), the phase state for all studied SOA precursors varied as a function of C SOA . Furthermore, the BF was found to be the maximum when SOA particle distributions reached a geometric mean particle diameter of 50-60 nm. Experimental results indicate that C SOA is an important parameter impacting the phase state of SOA, reinforcing recent findings that extrapolation of experiments not conducted at atmospherically relevant SOA levels may not yield results that are relevant to the natural environment.

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Section: Introductionmentioning

confidence: 99%

The Influence of Absolute Mass Loading of Secondary Organic Aerosols on Their Phase State

2018

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“…al., 2017b; Kanakidou et al, 2005;Pachauri et al, 2014;Pöschl and Shiraiwa, 2015). Characterizing these impacts crucially depends on our ability to determine and quantify aerosol sources and strengths (Bai et al, 2013;Robinson et al, 2006;McFiggans et al, 2019;Hopke, 2016), and to understand the physical and chemical transformation of aerosol particles during atmospheric transport by multiphase chemical processes (George and Abbatt, 2010;Rudich et al, 2007;Laskin et al, 2015;Springmann et al, 2009;Kaiser et al, 2011;Ervens et al, 2011;Zhou et al, 2019;Moise et al, 2015). Gas-to-particle, also termed heterogeneous, reactions can involve organic components in the condensed phase and gas-phase oxidants such as O 3 , NO 3, and OH.…”

Section: Introductionmentioning

confidence: 99%

“…Gas-to-particle, also termed heterogeneous, reactions can involve organic components in the condensed phase and gas-phase oxidants such as O 3 , NO 3, and OH. These reactions, which can include multiple phases, change the physicochemical properties of particles including composition, density, and hygroscopicity, thereby defining their chemical lifetime, optical properties, and ice nucleating ability (Jimenez et al, 2009;Kroll et al, 2015;Katrib et al, 2005b;Knopf et al, 2018;Slade et al, 2017;Robinson et al, 2007;Shiraiwa et al, 2017a;Moise et al, 2015;.…”

Section: Introductionmentioning

confidence: 99%

“…The phase state of OA can be modulated by particle composition and environmental conditions such as relative humidity (RH) and temperature (Koop et al, 2011;Zobrist et al, 2008;Shiraiwa et al, 2017a;Petters et al, 2019). Particle viscosity will influence the diffusion of atmospheric oxidants and other small gas molecules (e.g., O 3 , OH, NO 3 , H 2 O) entering the organic matrix (Price et al, 2015;Zobrist et al, 2011;Slade et al, 2017;Davies and Wilson, 2016;Moridnejad and Preston, 2016) as well as the transport and mixing of the condensed-phase organic species (Rothfuss and Petters, 2017;Marsh et al, 2018;Lienhard et al, 2015;Abramson et al, 2013;Chenyakin et al, 2017;Kiland et al, 2019). Therefore, it can be expected that the particle phase state will significantly affect the rate of multiphase chemical kinetics (Shiraiwa and Seinfeld, 2012;Slade and Knopf, 2014;Kolesar et al, 2014;Knopf et al, 2005;Katrib et al, 2005a;Davies and Wilson, 2015;Pöschl and Shiraiwa, 2015).…”

Section: Introductionmentioning

confidence: 99%

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Heterogeneous oxidation of amorphous organic aerosol surrogates by O3, NO3, and OH at typical tropospheric temperatures

Li¹,

Forrester²,

Knopf³

2020

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Abstract. Typical tropospheric temperatures render possible phase states of amorphous organic aerosol (OA) particles to solid, semi-solid and liquid. This will affect the multiphase oxidation kinetics involving the organic condensed phase and gaseous oxidants and radicals. To quantify this effect, we determined the reactive uptake coefficients (&#947;) of O3, NO3 and OH by substrate films composed of single and binary OA surrogate species under dry conditions for temperatures from 213 to 313&#8201;K. A temperature-controlled coated-wall flow reactor coupled to a chemical ionization mass spectrometer was applied to determine &#947; with consideration of gas diffusion transport limitation and gas flow entrance effects, which can impact heterogeneous reaction kinetics. The phase state of the organic substrates was probed via the poke-flow technique, allowing the estimation of the substrates&#8217; glass transition temperatures. &#947; values for O3 and OH uptake to a canola oil substrate, NO3 uptake to a levoglucosan and a levoglucosan/xylitol substrate, and OH uptake to a glucose and glucose/1,2,6-hexanetriol substrate have been determined as a function of temperature. We observed the greatest changes in &#947; with temperature for substrates that experienced the largest changes in viscosity as a result of a solid-to-liquid phase transition. Organic substrates that maintain a semi-solid or solid phase state and as such a relatively higher viscosity, do not display large variations in heterogeneous reactivity. From 213&#8201;K to 293&#8201;K, &#947; values of O3 with canola oil, of NO3 with a levoglucosan/xylitol mixture, and of OH with a glucose/1,2,6-hexanetriol mixture and canola oil, increase by about a factor of 34, 3, 2 and 5, respectively, due to a solid-to-liquid phase transition of the substrate. These results demonstrate that the surface and bulk lifetime of the OA surrogate species can significantly increase due to the slowed heterogeneous kinetics when OA species are solid or highly viscous in the middle and upper troposphere. This experimental study will further our understanding of the chemical evolution of OA particles with subsequent important consequences for source apportionment, air quality, and climate.

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“…The optical and chemical properties of clouds (and thus their radiative forcing) are directly related to the aerosol and precipitation chemistry (Seinfeld et al, 2016). Moreover, clouds represent reactors of multiphase chemistry, contributing to many chemical transformations that would otherwise not take place, or would proceed at much slower rates (Herrmann et al, 2015; 80 Lance et al, 2017;Ravishankara, 1997;Schurman et al, 2018;Slade et al, 2017). Understanding the sources and fate of nitrogenous species in BB-influenced clouds is particularly important to comprehensively assess the environmental impacts of BB.…”

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confidence: 99%

Isotopic Constraints on the Atmospheric Sources and Formation of Nitrogenous Species in Biomass-Burning-Influenced Clouds

Chang

Zhang

et al. 2018

Preprint

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The interpretation of tropospheric cloud formation rests on understanding the sources and processes affecting aerosol constituents of the atmosphere that are preserved in cloudwater. 25 However, this challenge is difficult to be quantitatively addressed based on the sole use of bulk chemical properties. Nitrogenous aerosols, mainly ammonium (NH4 + ) and nitrate (NO3 -), play an important role in tropospheric cloud formation. Here we collected cloudwater samples at the summit of Mt. Tai (1545 m above sea level) in Eastern China during a long-lasting biomass burning (BB) event, and measured for the first time the isotopic compositions (mean ± 1σ) of 30 cloudwater nitrogen species (δ 15 N-NH4 + = -6.53 ± 4.96‰, δ 15 N-NO3 -= -2.35 ± 2.00‰, δ 18 O-NO3 -= 57.80 ± 4.23‰), allowing insights into their sources and potential transformation mechanism within the clouds. Large contributions of BB to the cloudwater NH4 + (32.9 ± 4.6%) and NO3 -(28.2 ± 2.7%) inventories were confirmed through a Bayesian isotopic mixing model, coupled with our newly-developed computational quantum chemistry module. Despite an overall reduction in total 35 anthropogenic NOx emission due to effective emission control actions and stricter emission standards for vehicles, the observed cloud δ 15 N-NO3values suggest that NOx emissions from transportation may have exceeded emissions from coal combustion. δ 18 O-NO3values imply that the reaction of OH with NO2 is the dominant pathway of NO3formation (57 ± 11%), yet the Atmos. Chem. Phys. Discuss., https://doi.

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Cloud droplet activation through oxidation of organic aerosol influenced by temperature and particle phase state

Cited by 61 publications

References 47 publications

The Influence of Absolute Mass Loading of Secondary Organic Aerosols on Their Phase State

The Influence of Absolute Mass Loading of Secondary Organic Aerosols on Their Phase State

Heterogeneous oxidation of amorphous organic aerosol surrogates by O<sub>3</sub>, NO<sub>3</sub>, and OH at typical tropospheric temperatures

Isotopic Constraints on the Atmospheric Sources and Formation of Nitrogenous Species in Biomass-Burning-Influenced Clouds

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Cloud droplet activation through oxidation of organic aerosol influenced by temperature and particle phase state

Cited by 61 publications

References 47 publications

The Influence of Absolute Mass Loading of Secondary Organic Aerosols on Their Phase State

The Influence of Absolute Mass Loading of Secondary Organic Aerosols on Their Phase State

Heterogeneous oxidation of amorphous organic aerosol surrogates by O&lt;sub&gt;3&lt;/sub&gt;, NO&lt;sub&gt;3&lt;/sub&gt;, and OH at typical tropospheric temperatures

Isotopic Constraints on the Atmospheric Sources and Formation of Nitrogenous Species in Biomass-Burning-Influenced Clouds

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Heterogeneous oxidation of amorphous organic aerosol surrogates by O<sub>3</sub>, NO<sub>3</sub>, and OH at typical tropospheric temperatures