The Role of Cloud Processing for the Ice Nucleating Ability of Organic Aerosol and Coal Fly Ash Particles

Kilchhofer, Kevin; Mahrt, Fabian; Kanji, Zamin A.

doi:10.1029/2020jd033338

Cited by 13 publications

(10 citation statements)

References 93 publications

(280 reference statements)

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“…These observations suggest that the changes with time in absorptivity of secondary BrC from phenolic precursors are greater than the changes in hygroscopicity. It is noted that cloud droplet activation at supersaturation 24 as well as ice nucleating ability 98 will influence the relative contributions of the direct and indirect effects, so this will need to be explored to complete the understanding of cloud processing of phenolic precursors.…”

Section: ■ Introductionmentioning

confidence: 99%

Hygroscopicity of Secondary Brown Carbon Aerosol from Aqueous Photo-Oxidation of Phenolic Precursors

Betz

Calvert

Al-Mashala

et al. 2022

ACS Earth Space Chem.

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To understand the impact of light-absorbing organic aerosol, also called brown carbon (BrC), it is necessary to determine the extent to which the direct effect through aerosol− radiation interactions and the indirect effect through aerosol−cloud interactions change during its atmospheric residence time. Toward addressing this need, the light absorption and water uptake of secondary BrC aerosol produced from phenolic compounds, abundant biomass burning emissions, were measured. Phenol, catechol, and pyrogallol were selected to form a homologous series, varying in the number of hydroxyl substituents, and they were exposed to aqueous hydroxyl radical in a photoreactor, leading to the formation of secondary BrC. The absorptivity of the BrC was monitored by UV−vis spectroscopy; the hygroscopicity was determined using a hygroscopic tandem differential mobility analyzer. The absorptivity of the secondary BrC increased within 8 h of photo-oxidation and then began decreasing. After 24 h of photooxidation, at an atmospherically relevant OH exposure of 2.2 × 10 −10 mol s L −1 , the hygroscopicity parameters for BrC from phenol, catechol, and pyrogallol were similar, i.e., 0.13 ± 0.02, 0.10 ± 0.02, and 0.13 ± 0.02, respectively, so BrC from phenolic compounds exhibits similar water uptake regardless of the functionalization of the precursor. After 36 and 48 h of continued photo-oxidation, during which the product mixture exhibited further whitening, the hygroscopicity parameter of secondary BrC from catechol did not change. These observations suggest that the changes in absorptivity (related to the direct effect) of secondary BrC produced from phenolic precursors are greater than the changes in hygroscopicity (related to the indirect effect) upon atmospheric aging.

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Section: ■ Introductionmentioning

confidence: 99%

Hygroscopicity of Secondary Brown Carbon Aerosol from Aqueous Photo-Oxidation of Phenolic Precursors

Betz

Calvert

Al-Mashala

et al. 2022

ACS Earth Space Chem.

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“…We observed the evidence of OA acting as immersion freezing INPs at a temperature warmer than that reported in other studies, for instance, isoprene initialized secondary organic aerosol (SOA) was found to nucleate at temperatures <−30°C in the laboratory (Ignatius et al., 2016; Ladino et al., 2014), and naphthalene‐induced SOA, a surrogate of anthropogenic SOA types, showed higher ice nucleating efficiency than biogenic SOA (Charnawskas et al., 2017). Further, recent studies have suggested that the phase state is a key factor in determining the contribution of OA to INPs (Kilchhofer et al., 2021; Wagner et al., 2015, 2017). Biogenic SOA was previously reported to not show a glass transition, which is shown by anthropogenic SOA (Liu et al., 2016), indicating that the latter may be more likely to be solid under low RH and serve as INPs.…”

Section: Resultsmentioning

confidence: 99%

Evidence for Anthropogenic Organic Aerosols Contributing to Ice Nucleation

Tian

Liu

et al. 2022

Geophysical Research Letters

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Ice nucleation (IN) determines the microphysical properties of mixed-phase and cirrus clouds, thus exerting an important impact on weather and climate (Boucher et al., 2013;DeMott et al., 2010). Heterogeneous IN can occur above −38°C and requires ice nucleating particles (INPs) (Pruppacher & Klett, 1997), among which process immersion freezing from existing supercooled liquid water drops is the dominant mechanism for midlatitude precipitation (Mülmenstädt et al., 2015;Westbrook & Illingworth, 2013). Despite the important role of INPs, their atmospheric sources and abundance remain to be clarified in detail (Kanji et al., 2017;Seinfeld et al., 2016).The INPs refer to the immersion freezing mode unless otherwise stated in this study. The IN efficiency of particles is highly composition-dependent, and a few candidates are well established, including mineral dust (DeMott

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“…Deposition ice nucleation requires low ice supersaturation and temperature values which exclude haze particle or liquid droplet formation and homogeneous freezing. In addition to molecular composition, the trajectory of the particle along a thermodynamic path, and the glass transition temperature ( T g ), which is non‐equilibrium phase transition temperature from glassy solid‐phase to semi‐solid phase (Koop et al., 2011), are important modulators of the ice nucleating ability of a particle (e.g., Berkemeier et al., 2014; Charnawskas et al., 2017; Kilchhofer et al., 2021; Lienhard et al., 2015; Murray et al., 2010). When the glassy particle is exposed to an increase of RH, it starts to liquefy and form a core‐shell morphology then the water diffuses into the glassy matrix.…”

Section: Introductionmentioning

confidence: 99%

“…Many model organic species have been identified as IN active substances (Baustian et al., 2013; Gavish et al., 1990; Kilchhofer et al., 2021; Knopf et al., 2018; Murray et al., 2010; Rosinski et al., 1990; Wagner et al., 2010; Wolf et al., 2020). The reported observations show that particles composed of pure organic compounds such as sucrose (Baustian et al., 2013), raffinose (Kilchhofer et al., 2021; Wagner et al., 2012; Wilson et al., 2012), citric acid (Murray et al., 2010), and oxalic acid dihydrate (Wagner et al., 2010) nucleate ice in the heterogeneous regime. Deposition ice nucleation requires low ice supersaturation and temperature values which exclude haze particle or liquid droplet formation and homogeneous freezing.…”

Section: Introductionmentioning

confidence: 99%

Experimental Determination of the Relationship Between Organic Aerosol Viscosity and Ice Nucleation at Upper Free Tropospheric Conditions

et al. 2022

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Cirrus clouds play an important role in Earth's energy budget by reflecting the incoming solar radiation into space which leads to cooling, and by reducing the infrared longwave coming from the Earth surface which leads to warming (Chen et al., 2000;Heymsfield et al., 2017;Storelvmo & Herger, 2014). The radiative properties of cirrus clouds depend on the ice crystal number concentration, which in turn depends on the aerosol that nucleate ice at these conditions. Cirrus cloud ice crystals form either through homogeneous processes, requiring no ice nucleating particle (INP) or active site, or heterogeneously where an INP is involved (Hoose & Möhler, 2012;Kanji et al., 2017;Vali et al., 2015). Heterogeneous ice nucleation (IN) can occur via deposition of ice on particle surfaces, condensation in pores and subsequent freezing (Campbell et al., 2017;David et al., 2019;Marcolli, 2014), through immersion freezing of droplets as they cool, or condensation freezing as particles simultaneously uptake water and cool. Another freezing path is contact freezing where a particle approaches the air-water interface from either the outside of the droplet or from inside of the droplet (Durant & Shaw, 2005;Kanji et al., 2017). Homogeneous freezing of liquid aerosol is predominantly controlled by water activity (or ambient relative humidity (RH)), temperature, particle size, and hygroscopicity (Baumgartner et al., 2022;Koop et al., 2000;Schneider et al., 2021). Among these, temperature and RH dominate. Chemical composition influences homogeneous IN by modulating hygroscopicity (Junge, 1953;M. D. Petters & Kreidenweis, 2007). However, the overall influence of chemical composition on homogeneous freezing nucleation is small (Kreidenweis et al., 2009). In contrast, heterogeneous IN strongly depends on the chemical composition and morphology (Hiranuma et al., 2014). Ambient measurements of cirrus ice crystal residuals show a wide range of chemical composition, including organic particles, black carbon, mineral dust, lead and other metal bearing particles, sulfate particles, and salt particles

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The Role of Cloud Processing for the Ice Nucleating Ability of Organic Aerosol and Coal Fly Ash Particles

Cited by 13 publications

References 93 publications

Hygroscopicity of Secondary Brown Carbon Aerosol from Aqueous Photo-Oxidation of Phenolic Precursors

Hygroscopicity of Secondary Brown Carbon Aerosol from Aqueous Photo-Oxidation of Phenolic Precursors

Evidence for Anthropogenic Organic Aerosols Contributing to Ice Nucleation

Experimental Determination of the Relationship Between Organic Aerosol Viscosity and Ice Nucleation at Upper Free Tropospheric Conditions

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