Humidity-Dependent Viscosity of Secondary Organic Aerosol from Ozonolysis of β-Caryophyllene: Measurements, Predictions, and Implications

Maclean, Adrian M.; Smith, Natalie R.; Liu, Ying; Huang, Yuanzhou; Hettiyadura, Anusha P. S.; Crescenzo, Giuseppe V.; Shiraiwa, Manabu; Laskin, Alexander; Nizkorodov, Sergey A.; Bertram, Allan K.

doi:10.1021/acsearthspacechem.0c00296

Cited by 45 publications

(84 citation statements)

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“…Different types of SOAs generated in environmental chambers and flow reactors have been examined. The dynamic viscosities of some types of SOA particles (e.g., generated from toluene and diesel vapors) ranged from 10 −3 to 10 8 Pa s, which is approximately equal to the range of viscosities between that of water and tar pitch, depending on the RH, oxidation state, and chemical composition (Mikhailov et al, 2009;Virtanen et al, 2010;Vaden et al, 2011;Koop et al, 2011;Saukko et al, 2012;Renbaum-Wolff et al, 2013a;Hao et al, 2014;Kidd et al, 2014;Bateman et al, 2015;Athanasiadis et al, 2016;Grayson et al, 2016Grayson et al, , 2017Hinks et al, 2016;Hosny et al, 2016;Rothfuss and Petters, 2017;Yli-Juuti et al, 2017;Petters et al, 2019;Gervasi et al, 2020). In addition to the viscosity of SOA, the viscosity effects of inorganic salts should also be investigated to better understand the viscosities and phase states of atmospherically relevant mixed particles.…”

Section: Introductionmentioning

confidence: 96%

“…Most studies on this topic have focused on the determination of the viscosities and phase state of secondary organic aerosols (SOAs) (Mikhailov et al, 2009;Virtanen et al, 2010;Koop et al, 2011;Vaden et al, 2011;Saukko et al, 2012;Renbaum-Wolff et al, 2013;Hao et al, 2014;Kidd et al, 2014;Bateman et al, 2015;Athanasiadis et al, 2016;Grayson et al, 2016;Hinks et al, 2016;Hosny et al, 2016;Yli-Juuti et al, 2017;Petters et al, 2019;Wallace and Preston, 2019;Gervasi et al, 2020;Schmedding et al, 2020). Different types of SOAs generated in environmental chambers and flow reactors have been examined.…”

Section: Introductionmentioning

confidence: 99%

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Viscosity and phase state of aerosol particles consisting of sucrose mixed with inorganic salts

et al. 2021

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Abstract. Research on the viscosity and phase state of aerosol particles is essential because of their significant influence on the particle growth rate, equilibration times, and related evolution of mass concentration as well as heterogeneous reactions. So far, most studies of viscosity and phase state have been focused on organic aerosol particles, yet data on how viscosity can vary when the organic materials are mixed with inorganic salts remain scarce. Herein, using bead-mobility and poke-and-flow techniques, we quantified viscosities at 293 ± 1 K for binary mixtures of organic material / H2O and inorganic salts / H2O, as well as ternary mixtures of organic material / inorganic salts / H2O over the atmospheric relative humidity (RH) range. Sucrose as the organic species and calcium nitrate (Ca(NO3)2) or magnesium nitrate (Mg(NO3)2) as the inorganic salts were examined. For binary sucrose / H2O particles, the viscosities gradually increased from ∼ 3 × 10−2 to ≳1 × 108 Pa s as RH decreased from ∼ 75 % to ∼ 25 %. Compared with the results for the sucrose / H2O particles, binary Ca(NO3)2/H2O and Mg(NO3)2/H2O particles showed drastic enhancements to ≳1 × 108 Pa s at low RH close to the efflorescence RH. For ternary mixtures of sucrose / Ca(NO3)2 / H2O or sucrose / Mg(NO3)2 / H2O, with organic-to-inorganic mass ratios of 1:1, the viscosities of the particles gradually increased from ∼ 3 × 10−2 to greater than ∼ 1 × 108 Pa s for RH values from ∼ 75 % to ∼ 5 %. Compared to the viscosities of the Ca(NO3)2/H2O particles, higher viscosities were observed for the ternary sucrose / Ca(NO3)2 / H2O particles, with values increased by about 1 order of magnitude at 50 % RH and about 6 orders of magnitude at 35 % RH. Moreover, we applied a thermodynamics-based group-contribution model (AIOMFAC-VISC, Aerosol Inorganic–Organic Mixtures Functional groups Activity Coefficients Viscosity) to predict aerosol viscosities for the studied systems. The model predictions and viscosity measurements show good agreement within ∼ 1 order of magnitude in viscosity. The viscosity measurements indicate that the studied mixed organic–inorganic particles range in phase state from liquid to semi-solid or even solid across the atmospheric RH range at a temperature of 293 K. These results support our understanding that organic / inorganic / H2O particles can exist in a liquid, semisolid, or even a solid state in the troposphere.

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Section: Introductionmentioning

confidence: 96%

Section: Introductionmentioning

confidence: 99%

Viscosity and phase state of aerosol particles consisting of sucrose mixed with inorganic salts

et al. 2021

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“…For example, Grayson et al (2016) used the poke-and-flow technique to measure the viscosity of α-pinene derived SOA at CSOA between 120 and 14,000 μg m -3 . Maclean et al (2021) recently completed a similar poke-and-flow study with β-caryophyllene derived SOA. Kidd et al (2014) found similar results by studying SOA impaction patterns onto a germanium crystal, which also permitted FTIR spectroscopic analysis of chemical composition.…”

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confidence: 99%

Utilizing an Electrical Low Pressure Impactor to Indirectly Probe Water Uptake via Particle Bounce Measurements

Fischer

Petrucci

2021

Preprint

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Abstract. Secondary organic aerosol (SOA), formed through oxidation of volatile organic compounds (VOCs), display complex viscosity and phase behaviors influenced by temperature, relative humidity (RH), and chemical composition. Here, the efficacy of a multi-stage electrical low pressure impactor (ELPI) for indirect water uptake measurements was studied for ammonium sulfate (AS) aerosol, sucrose aerosol, and α-pinene derived SOA. All three aerosol systems were subjected to greater than 90 % chamber relative humidity, with subsequent analysis indicating persistence of particle bounce for sucrose 10 aerosol of 70 nm (initial dry diameter) and α-pinene derived SOA of number geometric mean diameters between 39 nm and 136 nm (initial dry diameter). On the other hand, sucrose aerosol of 190 nm (initial dry diameter) and AS aerosol down to 70 nm (initial dry diameter) exhibited no particle bounce at elevated RH. Partial drying of aerosol within the lower diameter ELPI impaction stages, where inherent and significant RH reductions occur, is proposed as one explanation for particle bounce persistence.

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“…Environmental factors, such as relative humidity and temperature, can influence the viscosity of the particle [4,5]. The effect of relative humidity on viscosity has been the focus of extensive studies over the past few decades [6][7][8][9][10]. In higher relative humidity conditions, the higher water content in the particle phase decreases the viscosity of the particle.…”

Section: Introductionmentioning

confidence: 99%

Temperature-Dependent Viscosity of Organic Materials Characterized by Atomic Force Microscope

Qin

Ohno

et al. 2021

Atmosphere

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The viscosity of atmospheric aerosol particles determines the equilibrium timescale at which a molecule diffuses into and out of particles, influencing processes such as gas–particle partitioning, light scattering, and cloud formation that can affect air quality and climate. This particle viscosity is sensitive to environmental conditions such as relative humidity and temperature. Current experimental techniques mainly characterize aerosol viscosity at room temperature. The influence of temperature on the viscosity of organic aerosol remains underexplored. Herein, the viscosity of atmospherically relevant organic materials was examined at a range of temperatures from 15 °C to 95 °C using an atomic force microscope (AFM) equipped with a temperature-controlled sample module. Dioctyl phthalate and sucrose were selected for investigation. Dioctyl phthalate served as the proxy for atmospherically relevant primary organic materials while sucrose served as the proxy for secondary organic materials. The resonant frequency responses of the AFM cantilever within dioctyl phthalate and sucrose were recorded. The link between the resonant frequency and material viscosity was established via a hydrodynamic function. Results obtained from this study were consistent with previously reported viscosities, thus demonstrating the critical capability of AFM in temperature-dependent viscosity measurements.

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Humidity-Dependent Viscosity of Secondary Organic Aerosol from Ozonolysis of β-Caryophyllene: Measurements, Predictions, and Implications

Cited by 45 publications

References 125 publications

Viscosity and phase state of aerosol particles consisting of sucrose mixed with inorganic salts

Viscosity and phase state of aerosol particles consisting of sucrose mixed with inorganic salts

Utilizing an Electrical Low Pressure Impactor to Indirectly Probe Water Uptake via Particle Bounce Measurements

Temperature-Dependent Viscosity of Organic Materials Characterized by Atomic Force Microscope

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