| 1. |
- Alsved, Malin, et al.
(author)
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Effect of Aerosolization and Drying on the Viability of Pseudomonas syringae Cells
- 2018
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In: Frontiers in Microbiology. - : Frontiers Media SA. - 1664-302X. ; 9
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Journal article (peer-reviewed)abstract
- Airborne dispersal of microorganisms influences their biogeography, gene flow, atmospheric processes, human health and transmission of pathogens that affect humans, plants and animals. The extent of their impact depends essentially on cell-survival rates during the process of aerosolization. A central factor for cell-survival is water availability prior to and upon aerosolization. Also, the ability of cells to successfully cope with stress induced by drying determines their chances of survival. In this study, we used the ice-nucleation active, plant pathogenic Pseudomonas syringae strain R10.79 as a model organism to investigate the effect of drying on cell survival. Two forms of drying were simulated: drying of cells in small droplets aerosolized from a wet environment by bubble bursting and drying of cells in large droplets deposited on a surface. For drying of cells both in aerosol and surface droplets, the relative humidity (RH) was varied in the range between 10 and 90%. The fraction of surviving cells was determined by live/dead staining followed by flow cytometry. We also evaluated the effect of salt concentration in the water droplets on the survival of drying cells by varying the ionic strength between 0 and 700 mM using NaCl and sea salt. For both aerosol and surface drying, cell survival increased with decreasing RH (p < 0.01), and for surface drying, survival was correlated with increasing salt concentration (p < 0.001). Imaging cells with TEM showed shrunk cytoplasm and cell wall damage for a large fraction of aerosolized cells. Ultimately, we observed a 10-fold higher fraction of surviving cells when dried as aerosol compared to when dried on a surface. We conclude that the conditions, under which cells dry, significantly affect their survival and thus their success to spread through the atmosphere and colonize new environments as well as their ability to affect atmospheric processes.
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| 2. |
- Christiansen, Sigurd, et al.
(author)
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Sea Spray Aerosol Formation : Laboratory Results on the Role of Air Entrainment, Water Temperature, and Phytoplankton Biomass
- 2019
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In: Environmental Science and Technology. - : American Chemical Society (ACS). - 0013-936X .- 1520-5851. ; 53:22, s. 13107-13116
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Journal article (peer-reviewed)abstract
- Sea spray aerosol (SSA) emission is a complex process affected by various controlling factors. This work seeks to deconvolute some of this complexity in a controlled laboratory setting using a plunging jet by varying three key parameters, one at a time: (1) air entrainment rate, (2) seawater temperature, and (3) biomass of phytoplankton. The production of SSA is found to vary linearly with air entrainment rate. By normalizing the production flux to air entrainment rate, we observe nonlinear variation of the production efficiency of SSA with seawater temperature with a minimum around 6-10 degrees C. For comparison, SSA was also generated by detraining air into artificial seawater using a diffuser demonstrating that the production efficiency of SSA generated using a diffuser decreases almost linearly with increasing seawater temperature, and the production efficiency is, significantly higher than that for SSA generated using a plunging jet. Finally, by varying the amount of phytoplankton biomass we demonstrate that SSA particle production varies nonlinearly with the amount of biomass in seawater.
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| 3. |
- Krieger, Ulrich K., et al.
(author)
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A reference data set for validating vapor pressure measurement techniques : homologous series of polyethylene glycols
- 2018
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In: Atmospheric Measurement Techniques. - : Copernicus GmbH. - 1867-1381 .- 1867-8548. ; 11:1, s. 49-63
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Journal article (peer-reviewed)abstract
- To predict atmospheric partitioning of organic compounds between gas and aerosol particle phase based on explicit models for gas phase chemistry, saturation vapor pressures of the compounds need to be estimated. Estimation methods based on functional group contributions require training sets of compounds with well-established saturation vapor pressures. However, vapor pressures of semivolatile and low-volatility organic molecules at atmospheric temperatures reported in the literature often differ by several orders of magnitude between measurement techniques. These discrepancies exceed the stated uncertainty of each technique which is generally reported to be smaller than a factor of 2. At present, there is no general reference technique for measuring saturation vapor pressures of atmospherically relevant compounds with low vapor pressures at atmospheric temperatures. To address this problem, we measured vapor pressures with different techniques over a wide temperature range for intercomparison and to establish a reliable training set. We determined saturation vapor pressures for the homologous series of polyethylene glycols (H-(O-CH2-CH2)(n)-OH) for n = 3 to n = 8 ranging in vapor pressure at 298 K from 10(-7) to 5 x 10(-2) Pa and compare them with quantum chemistry calculations. Such a homologous series provides a reference set that covers several orders of magnitude in saturation vapor pressure, allowing a critical assessment of the lower limits of detection of vapor pressures for the different techniques as well as permitting the identification of potential sources of systematic error. Also, internal consistency within the series allows outlying data to be rejected more easily. Most of the measured vapor pressures agreed within the stated uncertainty range. Deviations mostly occurred for vapor pressure values approaching the lower detection limit of a technique. The good agreement between the measurement techniques (some of which are sensitive to the mass accommodation coefficient and some not) suggests that the mass accommodation coefficients of the studied compounds are close to unity. The quantum chemistry calculations were about 1 order of magnitude higher than the measurements. We find that extrapolation of vapor pressures from elevated to atmospheric temperatures is permissible over a range of about 100 K for these compounds, suggesting that measurements should be performed best at temperatures yielding the highest-accuracy data, allowing subsequent extrapolation to atmospheric temperatures.
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| 4. |
- Kristensen, Kasper, et al.
(author)
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High-Molecular Weight Dimer Esters Are Major Products in Aerosols from α-Pinene Ozonolysis and the Boreal Forest
- 2016
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In: Environmental Science and Technology. - : American Chemical Society (ACS). - 0013-936X .- 1520-5851. ; 3:8, s. 280-285
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Journal article (peer-reviewed)abstract
- This study investigates the contribution of high-molecular weight dimer esters to laboratory-generated α-pinene gas- and particle-phase secondary organic aerosol (SOA) and particulate matter (PM) collected at the Nordic boreal forest site of Hyytiälä, Finland. Laboratory flow reactor experiments (25 °C) show that dimer esters from ozonolysis of α-pinene contribute between 5 and 16% of the freshly formed α-pinene particle-phase SOA mass. An increased level of formation is observed at a higher relative humidity of ∼40%, and the presence of a hydroxyl radical (OH) scavenger is shown to affect the formation of dimer esters. Of the 28 dimer esters identified in laboratory α-pinene SOA, 15 are also observed in ambient PM samples, contributing between 0.5 and 1.6% of the total PM1. The observed esters show good correlation with known α-pinene SOA tracers in collected PM samples. This work reveals an, until now, unrecognized contribution of dimer esters from α-pinene oxidation to boreal forest PM.
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| 5. |
- Quelever, Lauriane L.J., et al.
(author)
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Effect of temperature on the formation of highly oxygenated organic molecules (HOMs) from alpha-pinene ozonolysis
- 2019
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In: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 19:11, s. 7609-7625
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Journal article (peer-reviewed)abstract
- Highly oxygenated organic molecules (HOMs) are important contributors to secondary organic aerosol (SOA) and new-particle formation (NPF) in the boreal atmosphere. This newly discovered class of molecules is efficiently formed from atmospheric oxidation of biogenic volatile organic compounds (VOCs), such as monoterpenes, through a process called autoxidation. This process, in which peroxy-radical intermediates isomerize to allow addition of molecular oxygen, is expected to be highly temperature-dependent. Here, we studied the dynamics of HOM formation during α-pinene ozonolysis experiments performed at three different temperatures, 20, 0 and -15 ĝC, in the Aarhus University Research on Aerosol (AURA) chamber. We found that the HOM formation, under our experimental conditions (50 ppb α-pinene and 100 ppb ozone), decreased considerably at lower temperature, with molar yields dropping by around a factor of 50 when experiments were performed at 0 ĝC, compared to 20 ĝC. At -15 ĝC, the HOM signals were already close to the detection limit of the nitrate-based chemical ionization atmospheric pressure interface time-of-flight (CI-APi-TOF) mass spectrometer used for measuring gas-phase HOMs. Surprisingly, comparing spectra measured at 0 and 20 ĝC, ratios between HOMs of different oxidation levels, e.g., the typical HOM products C10H14O7, C10H14O9, and C10H14O11, changed considerably less than the total HOM yields. More oxidized species have undergone more isomerization steps; yet, at lower temperature, they did not decrease more than the less oxidized species. One possible explanation is that the primary rate-limiting steps forming these HOMs occur before the products become oxygenated enough to be detected by our CI-APi-TOF (i.e., typically seven or more oxygen atoms). The strong temperature dependence of HOM formation was observed under temperatures highly relevant to the boreal forest, but the exact magnitude of this effect in the atmosphere will be much more complex: the fate of peroxy radicals is a competition between autoxidation (influenced by temperature and VOC type) and bimolecular termination pathways (influenced mainly by concentration of reaction partners). While the temperature influence is likely smaller in the boreal atmosphere than in our chamber, both the magnitude and complexity of this effect clearly deserve more consideration in future studies in order to estimate the ultimate role of HOMs on SOA and NPF under different atmospheric conditions.
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