To predict important secondary organic aerosol (SOA) properties, information on viscosity or diffusion rates within SOA is needed. Ozonolysis of β-caryophyllene is an important SOA source; however, very few viscosity or diffusion rate measurements have been performed for this SOA type and none as a function of relative humidity (RH). In this study, we measured viscosity as a function of RH for SOA generated from the ozonolysis of β-caryophyllene using the poke-flow technique. At an RH of 0 and 48%, the viscosity was between 6.9 × 105 and 2.4 × 107 Pa s, and between 1.3 × 103 and 5.6 × 104 Pa s, respectively. Based on these viscosities and the fractional Stokes–Einstein equation, characteristic mixing timescales of organics within 200 nm β-caryophyllene SOA particles range from ∼0.2 h at 0% RH to <3 s at 48% RH, suggesting that these particles should be well-mixed under most conditions in the lower atmosphere. The chemical composition of the SOA was also determined using nano-desorption electrospray ionization mass spectrometry. The measured chemical composition and the method of DeRieux et al. (ACP, 2018) were used to predict the viscosity of β-caryophyllene SOA. If the mass spectra peak abundances were adjusted to account for the sensitivity of the electrospray ionization to larger molecular weight components, the predicted viscosity overlapped with the measured viscosity at 0% RH, while the predicted viscosities at 15–48% RH were slightly higher than the measured viscosities. The measured viscosities also overlapped with viscosity predictions based on a simple mole-fraction based Arrhenius mixing rule.
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.
Abstract. Information on liquid–liquid phase separation (LLPS) and viscosity (or diffusion) within secondary organic aerosol (SOA) is needed to improve predictions of particle size, mass, reactivity, and cloud nucleating properties in the atmosphere. Here we report on LLPS and viscosities within SOA generated by the photooxidation of diesel fuel vapors. Diesel fuel contains a wide range of volatile organic compounds, and SOA generated by the photooxidation of diesel fuel vapors may be a good proxy for SOA from anthropogenic emissions. In our experiments, LLPS occurred over the relative humidity (RH) range of ∼70 % to ∼100 %, resulting in an organic-rich outer phase and a water-rich inner phase. These results may have implications for predicting the cloud nucleating properties of anthropogenic SOA since the presence of an organic-rich outer phase at high-RH values can lower the supersaturation with respect to water required for cloud droplet formation. At ≤10 % RH, the viscosity was ≥1×108 Pa s, which corresponds to roughly the viscosity of tar pitch. At 38 %–50 % RH, the viscosity was in the range of 1×108 to 3×105 Pa s. These measured viscosities are consistent with predictions based on oxygen to carbon elemental ratio (O:C) and molar mass as well as predictions based on the number of carbon, hydrogen, and oxygen atoms. Based on the measured viscosities and the Stokes–Einstein relation, at ≤10 % RH diffusion coefficients of organics within diesel fuel SOA is ≤5.4×10-17 cm2 s−1 and the mixing time of organics within 200 nm diesel fuel SOA particles (τmixing) is 50 h. These small diffusion coefficients and large mixing times may be important in laboratory experiments, where SOA is often generated and studied using low-RH conditions and on timescales of minutes to hours. At 38 %–50 % RH, the calculated organic diffusion coefficients are in the range of 5.4×10-17 to 1.8×10-13 cm2 s−1 and calculated τmixing values are in the range of ∼0.01 h to ∼50 h. These values provide important constraints for the physicochemical properties of anthropogenic SOA.
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.
The paediatric intensive care unit (PICU) provides care to critically ill neonates, infants and children. These patients are vulnerable and susceptible to the environment surrounding them, yet there is little information available on indoor air quality and factors affecting it within a PICU. To address this gap in knowledge we conducted continuous indoor and outdoor airborne particle concentration measurements over a two-week period at the Royal Children's Hospital PICU in Brisbane, Australia, and we also collected 82 bioaerosol samples to test for the presence of bacterial and viral pathogens. Our results showed that both 24-hour average indoor particle mass (PM) (0.6-2.2μgm, median: 0.9μgm) and submicrometer particle number (PN) (0.1-2.8×10pcm, median: 0.67×10pcm) concentrations were significantly lower (p<0.01) than the outdoor concentrations (6.7-10.2μgm, median: 8.0μgm for PM and 12.1-22.2×10pcm, median: 16.4×10pcm for PN). In general, we found that indoor particle concentrations in the PICU were mainly affected by indoor particle sources, with outdoor particles providing a negligible background. We identified strong indoor particle sources in the PICU, which occasionally increased indoor PN and PM concentrations from 0.1×10 to 100×10pcm, and from 2μgm to 70μgm, respectively. The most substantial indoor particle sources were nebulization therapy, tracheal suction and cleaning activities. The average PM and PN emission rates of nebulization therapy ranged from 1.29 to 7.41mgmin and from 1.20 to 3.96pmin×10, respectively. Based on multipoint measurement data, it was found that particles generated at each location could be quickly transported to other locations, even when originating from isolated single-bed rooms. The most commonly isolated bacterial genera from both primary and broth cultures were skin commensals while viruses were rarely identified. Based on the findings from the study, we developed a set of practical recommendations for PICU design, as well as for medical and cleaning staff to mitigate aerosol generation and transmission to minimize infection risk to PICU patients.
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