Abstract. Relationships between critical supersaturation required for activation and particle dry diameter have been the primary means for experimentally characterizing cloud condensation nuclei (CCN) activity; however, use of the dry diameter inherently limits the application to cases where the dry diameter can be used to accurately estimate solute volume. This study challenges the requirement and proposes a new experimental approach, Wet CCN, for studying CCN activity without the need for a drying step. The new approach directly measures the subsaturated portion of the Köhler curves. The experimental setup consists of a humidity-controlled differential mobility analyzer and a CCN counter; wet diameter equilibrated at known relative humidity is used to characterize CCN activity instead of the dry diameter. The experimental approach was validated against ammonium sulfate, glucose, and nonspherical ammonium oxalate monohydrate. Further, the approach was applied to a mixture of nonspherical iodine oxide particles. The Wet CCN approach successfully determined the hygroscopicity of nonspherical particles by collapsing them into spherical, deliquesced droplets. We further show that the Wet CCN approach offers unique insights into the physical and chemical impacts of the aqueous phase on CCN activity; a potential application is to investigate the impact of evaporation/co-condensation of water-soluble semivolatile species on CCN activity.
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Cloud condensation nuclei (CCN) activity analysis of low-hygroscopicity aerosols using the aerodynamic aerosol classifier (AAC)
Abstract. The aerodynamic aerosol classifier (AAC) is a novel instrument that size-selects aerosol particles based on their mechanical mobility. So far, the application of an AAC for cloud condensation nuclei (CCN) activity analysis of aerosols has yet to be explored. Traditionally, a differential mobility analyzer (DMA) is used for aerosol classification in a CCN experimental setup. A DMA classifies particles based on their electrical mobility. Substituting the DMA with an AAC can eliminate multiple-charging artifacts as classification using an AAC does not require particle charging. In this work, we describe an AAC-based CCN experimental setup and CCN analysis method. We also discuss and develop equations to quantify the uncertainties associated with aerosol particle sizing. To do so, we extend the AAC transfer function analysis and calculate the measurement uncertainties of the aerodynamic diameter from the resolution of the AAC. The analysis framework has been packaged into a Python-based CCN Analysis Tool (PyCAT 1.0) open-source code, which is available on GitHub for public use. Results show that the AAC size-selects robustly (AAC resolution is 10.1, diffusion losses are minimal, and particle transmission is high) at larger aerodynamic diameters (≥∼ 85 nm). The size-resolved activation ratio is ideally sigmoidal since no charge corrections are required. Moreover, the uncertainties in the critical particle aerodynamic diameter at a given supersaturation can propagate through droplet activation, and the subsequent uncertainties with respect to the single-hygroscopicity parameter (κ) are reported. For a known aerosol such as sucrose, the κ derived from the critical dry aerodynamic diameter can be up to ∼ 50 % different from the theoretical κ. In this work, we do additional measurements to obtain dynamic shape factor information and convert the sucrose aerodynamic to volume equivalent diameter. The volume equivalent diameter applied to κ-Köhler theory improves the agreement between measured and theoretical κ. Given the limitations of the coupled AAC–CCN experimental setup, this setup is best used for low-hygroscopicity aerosol (κ≤0.2) CCN measurements.
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- Award ID(s):
- 1708337
- PAR ID:
- 10318473
- Date Published:
- Journal Name:
- Atmospheric Measurement Techniques
- Volume:
- 15
- Issue:
- 4
- ISSN:
- 1867-8548
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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An instrumental trifecta now exists for aerosol separation and classification by aerodynamic diameter (Dae), mobility diameter (Dm) and mass (m) utilizing an aerodynamic aerosol classifier (AAC), differential mobility analyzer (DMA) and aerosol particle mass analyzer (APM), respectively. In principle, any combination of two measurements yields the third. These quantities also allow for the derivation of the particle effective density (ρeff) and dynamic shape factor (χ). Measured and/or derived deviations between tandem measurements are dependent upon the configuration but are generally less than 10 %. Notably, non-physical values of χ (< 1) and ρeff (> bulk) were determined by the AAC-APM. Harmonization of the results requires the use of χ in the determination of m and Dm from the AAC-DMA and AAC-APM requiring either a priori assumptions or determination from another method. Further errors can arise from assuming instead of measuring physical conditions – e.g. temperature and pressure affect the gas viscosity, mean free path and the Cunningham slip correction factor therefore impacting Dm, Dae – but are expected to have a smaller impact than χ. Utilizing this triplet of instrumentation in combination allows for quantitative determination of χ and the particle density (ρp). If the bulk density is known or assumed, then the packing density can be determined. The χ and ρp were determined to be 1.10 ± 0.03 and (1.00 ± 0.02) g cm-3, respectively, for a water stabilized black carbon mimic that resembles aged (collapsed) soot in the atmosphere. Assuming ρbulk = 1.8 g cm 3, a packing density of 0.55 ± 0.02 is obtained.more » « less
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