Interactions of organosulfates with water vapor under sub- and supersaturated conditions

Organosulfates (OS) are important constituents of secondary organic aerosols, but their hygroscopic properties and cloud condensation nucleation (CCN) activities have not been well understood. In this work we employed three complementary techniques to characterize interactions of several OS with water vapor under sub- and supersaturated conditions. A vapor sorption analyzer was used to measure mass changes of OS samples with RH (0–90 %); among the 11 organosulfates examined, only sodium methyl sulfate (methyl-OS), sodium ethyl sulfate (ethyl-OS), sodium octyl sulfate (octyl-OS) and potassium hydroxyacetone sulfate were found to deliquesce as RH increased, and their mass growth factors at 90 % RH were determined to be 3.652 ± 0.064, 3.575 ± 0.024, 1.591 ± 0.004 and 2.202 ± 0.031. Hygroscopic growth of methyl-, ethyl- and octyl-OS aerosols was also studied using a humidity tandem differential mobility analyzer (H-TDMA); continuous hygroscopic growth was observed, and their growth factors at 90 % RH were determined to be 1.83 ± 0.03, 1.79 ± 0.02 and 1.21 ± 0.02. We further investigated CCN activities of methyl-, ethyl- and octyl-OS aerosols, and their single hygroscopicity parameters (κccn) were determined to be 0.459 ± 0.021, 0.397 ± 0.010 and 0.206 ± 0.008. For methyl- and ethyl-OS aerosols, κccn values agree reasonably well with those derived from H-TDMA measurements (κgf), whereas κccn was found to be significantly larger than κgf for octyl-OS, likely due to both solubility limit and surface tension reduction.

Laboratory Measurements of the Size Distribution and Activation Ratio of Synthetic Ice Nuclei

<p>Laboratory measurement of the particle size distribution and cloud condensation nucleation activation ratio are conducted using two types of synthetic ice nuclei (IN). New Engineered Organic Nuclei (NEON) are fabricated by fermentation and so-called E-lysis of Gram-negative bacteria, which are havested via centrifugation and resuspended in a NaHCO<sub>3</sub> buffer (pH of ~7.8) for final inactivation of lysis escape muntants. NEON is inactivated using 1.25 % (final concentration) glutaraldehyde (GA) and stored in a deep freezer. The NEON with GA solution is atomized using a Sparging Liquid Aerosol Generator (SLAG), which does not sheer or impact the aerosols. The measured size distribution is compared to aerosols produced by the TSI Atmomizer (Model 3076), which impacts generated droplets. The size distribution is measured using a TSI Scanning Mobility Particle Sizer Spectrometer (SMPS) and a TSI Aerodynamic Particle Sizer. A DMT Cloud Condensation Nuclei Counter (CCNC) operated at 0.6 % supersaturation and a TSI Condensation Particle Counter (CPC) is used to measure the activation ratio, which is important to determine effectiveness of the NEON as an immersion ice nuclei. The NEON results are compared to IN produced by burning silver iodine cloud seeding flares.</p>

A thermodynamic description for the hygroscopic growth of atmospheric aerosol particles

The phase state of atmospheric particulate is important to atmospheric processes, and aerosol radiative forcing remains a large uncertainty in climate predictions. That said, precise atmospheric phase behavior is difficult to quantify and observations have shown that “precondensation” of water below predicted saturation values can occur. We propose a revised approach to understanding the transition from solid soluble particles to liquid droplets, typically described as cloud condensation nucleation – a process that is traditionally captured by Köhler theory, which describes a modified equilibrium saturation vapor pressure due to (i) mixing entropy (Raoult's law) and (ii) droplet geometry (Kelvin effect). Given that observations of precondensation are not predicted by Köhler theory, we devise a more complete model that includes interfacial forces giving rise to predeliquescence, i.e., the formation of a brine layer wetting a salt particle at relative humidities well below the deliquescence point.

A thermodynamic description for the hygroscopic growth of atmospheric aerosol particles

The phase state of atmospheric particulate is important to atmospheric processes and aerosol radiative forcing remains a large uncertainty in climate predictions. That said, precise atmospheric phase behavior is difficult to quantify and observations have shown that precondensation of water below predicted saturation values can occur. We propose a revised approach to understanding the transition from solid soluble particles to liquid droplets, typically described as cloud condensation nucleation – a process that is traditionally captured by Köhler theory, which describes a modified equilibrium saturation vapor pressure due to I. mixing entropy (Raoult's law) and II. droplet geometry (Kelvin effect). Given that observations of precondensation are not predicted by Köhler theory, we devise a more complete model which includes interfacial forces giving rise to predeliquescence, i.e., the formation of a brine layer wetting a salt particle at relative humidities well below the deliquescence point.