Cloud condensation nuclei (CCN) activity analysis of low-hygroscopicity aerosols using the aerodynamic aerosol classifier (AAC)

Abstract

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.

Kinetic Limitations Affect Cloud Condensation Nuclei Activity Measurements Under Low Supersaturation

“…The CCN activity of aerosols, namely the fraction of particles activated into cloud droplets, can be directly measured by the continuous‐flow streamwise thermal‐gradient CCN counter (CCNC). The most commonly used CCNC was developed and commercialized by Droplet Measurement Technologies (DMT) (Lance et al., 2006; Roberts & Nenes, 2005), which has been widely applied in both field observation and laboratory experiment of aerosol CCN activity (Gohil & Asa‐Awuku, 2022; Kerminen et al., 2012; Kuang, Xu, et al., 2020; Paramonov et al., 2015; Tomi Raatikainen et al., 2013). This instrument consists of a continuous flow tube in which the walls are kept saturated with water and a positive wall temperature gradient is maintained.…”

“…Using the default cut off, however, can lead to 30% overestimation of the bulk CCN number concentration measurements for SS lower than 0.1% as unactivated particles might be counted (Yang et al., 2012). In addition, size‐resolved CCN activity measurements were widely performed for accurate CCN number predictions and model validation, and the data were also used to derive aerosol hygroscopicity parameter κ under supersaturated conditions (Deng et al., 2011; Gohil & Asa‐Awuku, 2022; Liu et al., 2018; Moore et al., 2010; Petters & Kreidenweis, 2007). There might be large deviations in retrieved aerosol hygroscopicity if the size‐resolved CCN activation curve was biased because of the misidentified CCN within specific diameter ranges.…”

A Single Parameter Hygroscopicity Model for Functionalized and Insoluble Aerosol Surfaces

“…In traditional Köhler (TK) theory, the droplet is assumed to be dilute, and the water activity follows Raoult's law; such that the water 35 activity equals the water mole fraction, and the dilute droplet water activity coefficient is assumed to be unity. For water-soluble particles like inorganic ammonium sulfate (Rose et al, 2008) and sucrose (Dawson et al, 2020;Gohil and Asa-Awuku, 2022), TK can accurately predict their water uptake behavior. However, TK does not work so well for atmospherically relevant and abundant particles that are partially water soluble or water insoluble (Kumar et al, 2009;Tang et al, 2016).…”

“…The droplet formation of water-insoluble particles has been previously described with adsorption activation models (Hatch et al, 2012;Kumar et al, 2009;Lintis et al, 2021;Malek et al, 2022;Navea et al, 2017;Pajunoja et al, 2015;Tang et al, 2016). Brunauer, Emmett, and Teller (BET) adsorption isotherm models are typically applied for multilayer adsorption analysis of water uptake on clays (Hatch et al, 2012) 45 and fly ash (Navea et al, 2017). Lintis et al, 2021 applied the Dubinin-Serpinsky model for soot and concluded that nucleation occurred at oxidized and hydrophilic surface sites on the soot.…”

“…Hatch et al, 2014 measured 60 montmorillonite dust and found that the AFHH and BFHH was 98 ± 22 and 1.79 ± 0.11 and the AFHH and BFHH was 75 ± 17 and 1.77 ± 0.11 for illite, respectively. Particles of intermediate polarity and high porosity may lead to a higher CCN activity (Koehler et al, 2009) and Hatch et al, 2012 attributed the high value of AFHH to the surface chemistry and the porosity of the clays. Specifically, porosity leads to a higher perceived hygroscopicity because water molecules fill the 65 microporous structure.…”