Viscosity and liquid–liquid phase separation in healthy and stressed plant SOA

Smith, Natalie R.; Crescenzo, Giuseppe V.; Huang, Yuanzhou; Hettiyadura, Anusha P. S.; Siemens, Kyla; Liu, Ying; Faiola, Celia; Laskin, Alexander; Shiraiwa, Manabu; Bertram, Allan K.; Nizkorodov, Sergey A.

doi:10.1039/d0ea00020e

Cited by 25 publications

(60 citation statements)

References 127 publications

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“…2a), but the viscosity values of the sucrose/AS/H2O particles at this OIR are approximately two orders of magnitude lower than those of sucrose/H2O particles at the same RH. In addition, the finding of gradual enhancements in the organic-rich particle is in consistent with the result of other recent viscosity studies of SOA particles (Song et al, 2015;Grayson et al, 2016;Hosny et al, 2016;Song et al, 2016a;Song et al, 2019;Gervasi et al, 2020;Maclean et al, 2021;Smith et al, 2021). The viscosities of the sucrose/AS/H2O for OIR = 4:1 corresponds to liquid for RH > ~52%, semisolid for ~18% < RH < ~50%, and semisolid or solid for RH < ~18%.…”

Section: Viscosities In Ternary Systems Of Sucrose/as/h2o With Differ...supporting

confidence: 91%

“…3b). Previous studies have shown such behaviour that organic-rich or SOA particles also cracked upon poking, without the appearance of crystallization (Song et al, 2019;Song et al, 2021;Smith et al, 2021). In particles consisting sucrose/AS/H2O particles with an OIR = 1:1, the mean viscosity varied from ~1 × 10 -2 to ~4 × 10 1 Pa‧s from ~70% to ~34% RH (yellow symbols in Fig.…”

Section: Viscosities In Ternary Systems Of Sucrose/as/h2o With Differ...mentioning

confidence: 84%

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Viscosity and physical state of sucrose mixed with ammonium sulfate droplets

Jeong

Lilek

Zuend

et al. 2022

Preprint

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Abstract. Although knowledge of the physical state of aerosol particles is essential to understand atmospheric chemistry model and measurements, information on the viscosity and physical state of aerosol particles consisting of organic and inorganic salts are still rare. Herein, we quantified viscosities at 293 ± 1 K upon dehydration for the binary systems, sucrose/H2O and ammonium sulfate (AS)/H2O, and the ternary systems, sucrose/AS/H2O for organic-to-inorganic dry mass ratios (OIRs) = 4 : 1, 1 : 1, and 1 : 4. For binary systems, the viscosity of sucrose/H2O particles gradually increased from ~6 × 10−1 to > ~1 × 108 Pa‧s when the relative humidity (RH) decreased from ~83 % to ~24 %, which agrees with previous studies. The viscosity of AS/H2O particles remained in the liquid state (< 102 Pa‧s) for RH > ~50 %, and for RH ≤ ~50 %, the particles showed viscosity of > ~1 × 1012 Pa‧s, corresponding to a solid state. For ternary systems, the viscosity of organic-rich particles (OIR = 4 : 1) gradually increased from ~4 × 10−2 to ~1 × 108 Pa‧s for a RH decrease from ~80 % to ~18 %, similar to the sucrose/H2O particles. In the particles for OIR = 1 : 1, the viscosities ranged smaller than ~4 × 101 for RH > 34 %, and > ~1 × 108 Pa‧s at ~27 % RH. Compared to the organic-rich particles, in the inorganic-rich particles (OIR = 1 : 4), drastic enhancement in viscosity was observed as RH decreased; the viscosity enhanced approximately 8 orders of magnitude in RH from 43 % to 25 %. Based on viscosity data, all particles studied in this work were observed to exist as a liquid, semi-solid or solid depending on the RH. Furthermore, we compared the measured viscosities of ternary systems with OIRs of 4 : 1, 1 : 1, and 1 : 4 to the predicted viscosities using the Aerosol Inorganic–Organic Mixtures Functional groups Activity Coefficients Viscosity model (AIOMFAC-VISC) predictions with the Zdanovskii–Stokes–Robinson (ZSR)-style organic–inorganic mixing model, with excellent model–measurement agreement for all OIRs.

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Section: Viscosities In Ternary Systems Of Sucrose/as/h2o With Differ...supporting

confidence: 91%

Section: Viscosities In Ternary Systems Of Sucrose/as/h2o With Differ...mentioning

confidence: 84%

Viscosity and physical state of sucrose mixed with ammonium sulfate droplets

Jeong

Lilek

Zuend

et al. 2022

Preprint

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“…We developed a parameterization for the viscosity of simulated pine tree SOA as a function of RH and temperature using the following data: (1) measured room-temperature viscosity data of SOA generated by the photooxidation of a mixture of volatile organic compounds (VOCs) representing emissions from healthy Scots pine (Pinus sylvestris) trees and (2) room-temperature viscosity data of water . These data are shown in Figure a.…”

Section: Materials and Methodsmentioning

confidence: 99%

“…The measured viscosities for the simulated Scots pine tree SOA at RH values less than or equal to 50% were taken from Smith et al, while the measured viscosities at RHs greater than 50% are based on new measurements discussed in the Supporting Information (Sections S1 and S2). The measured viscosities from Smith et al were based on the poke-flow technique, and the new measurements reported in the Supporting Information were based on the poke-flow technique and fluorescence recovery after photobleaching (FRAP). To determine viscosities from the poke-flow measurements, we used fluid simulations, which require material properties such as surface tension and slip length as the input .…”

Section: Materials and Methodsmentioning

confidence: 99%

“…However, these parameters are often not well constrained for the SOA material. As a result, conservative values were used in the simulations, which result in relatively large uncertainties in the viscosity data (Figure a) . The FRAP technique involved measuring diffusion coefficients of a large fluorescent dye within the SOA material and then converting these values to viscosity using the Stokes–Einstein equation.…”

Section: Materials and Methodsmentioning

confidence: 99%

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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

Maclean

Liu

Crescenzo

et al. 2021

ACS Earth Space Chem.

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Information on the global distributions of secondary organic aerosol (SOA) phase state and mixing times within SOA is needed to predict the impact of SOA on air quality, climate, and atmospheric chemistry; nevertheless, such information is rare. In this study, we developed parameterizations for viscosity as a function of relative humidity (RH) and temperature based on room-temperature viscosity data for simulated pine tree SOA and toluene SOA. The viscosity parameterizations were then used together with tropospheric RH and temperature fields to predict the SOA phase state and mixing times of water and organic molecules within SOA in the troposphere for 200 nm particles. Based on our results, the glassy state can often occur, and the mixing times of water can often exceed 1 h within SOA at altitudes >6 km. Furthermore, the mixing times of organic molecules within SOA can often exceed 1 h throughout most of the free troposphere (i.e., ≳1 km in altitude). In most of the planetary boundary layer (i.e., ≲1 km in altitude), the glassy state is not important, and the mixing times of water and organic molecules are less than 1 h. Our results are qualitatively consistent with the results from Shiraiwa et al. (Nat. Commun., 2017), although there are quantitative differences. Additional studies are needed to better understand the reasons for these differences.

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Observational Insights into Isoprene Secondary Organic Aerosol Formation through the Epoxide Pathway at Three Urban Sites from Northern to Southern China

Zhang

Ding

et al. 2022

Environ. Sci. Technol.

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Isoprene is the most abundant precursor of global secondary organic aerosol (SOA). The epoxide pathway plays a critical role in isoprene SOA (iSOA) formation, in which isoprene epoxydiols (IEPOX) and/or hydroxymethyl-methyl-α-lactone (HMML) can react with nucleophilic sulfate and water producing isoprene-derived organosulfates (iOSs) and oxygen-containing tracers (iOTs), respectively. This process is complicated and highly influenced by anthropogenic emissions, especially in the polluted urban atmospheres. In this study, we took a 1-year measurement of the paired iOSs and iOTs formed through the IEPOX and HMML pathways at the three urban sites from northern to southern China. The annual average concentrations of iSOA products at the three sites ranged from 14.6 to 36.5 ng m–3. We found that the nucleophilic–addition reaction of isoprene epoxides with water dominated over that with sulfate in the polluted urban air. A simple set of reaction rate constant could not fully describe iOS and iOT formation everywhere. We also found that the IEPOX pathway was dominant over the HMML pathway over urban regions. Using the kinetic data of IEPOX to estimate the reaction parameters of HMML will cause significant underestimation in the importance of HMML pathway. All these findings provide insights into iSOA formation over polluted areas.

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Viscosity and liquid–liquid phase separation in healthy and stressed plant SOA

Abstract: Molecular composition, viscosity, and phase state were investigated for secondary organic aerosol derived from synthetic mixtures of volatile organic compounds representing emissions from healthy and aphid-stressed Scots pine trees.

Cited by 25 publications

References 127 publications

Viscosity and physical state of sucrose mixed with ammonium sulfate droplets

Viscosity and physical state of sucrose mixed with ammonium sulfate droplets

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

Observational Insights into Isoprene Secondary Organic Aerosol Formation through the Epoxide Pathway at Three Urban Sites from Northern to Southern China

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