The size-resolved cloud condensation nuclei (CCN) activity and its prediction based on aerosol hygroscopicity and composition in the Pearl Delta River (PRD) region during wintertime 2014

A hygroscopic tandem differential mobility analyzer (HTDMA), a scanning mobility cloud condensation nuclei (CCN) analyzer (SMCA), and an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) were used to, respectively, measure the hygroscopicity, condensation nuclei activation, and chemical composition of aerosol particles at the Panyu site in the Pearl River Delta region during wintertime 2014. The distribution of the size-resolved CCN at four supersaturations (SSs of inline-formula0.1 %, 0.2 %, 0.4 %, and 0.7 %) and the aerosol particle size distribution were obtained by the SMCA. The hygroscopicity parameter inline-formulaκ (inline-formulaκ_CCN, inline-formulaκ_HTDMA, and inline-formulaκ_AMS) was, respectively, calculated based upon the SMCA, HTDMA, and AMS measurements. The results showed that the inline-formulaκ_HTDMA value was slightly smaller than the inline-formulaκ_CCN one at all diameters and for particles larger than 100 nm, and the inline-formulaκ_AMS value was significantly smaller than the others (inline-formulaκ_CCN and inline-formulaκ_HTDMA), which could be attributed to the underestimated hygroscopicity of the organics (inline-formulaκ_org). The activation ratio (AR) calculated from the growth factor – probability density function (Gf-PDF) without surface tension correction was found to be lower than that from the CCN measurements, due most likely to the uncorrected surface tension (inline-formulaσ_s∕a) that did not consider the surfactant effects of the organic compounds. We demonstrated that better agreement between the calculated and measured ARs could be obtained by adjusting inline-formulaσ_s∕a. Various schemes were proposed to predict the CCN number concentration (inline-formulaN_CCN) based on the HTDMA and AMS measurements. In general, the predicted inline-formulaN_CCN agreed reasonably well with the corresponding measured ones using different schemes. For the HTDMA measurements, the inline-formulaN_CCN value predicted from the real-time AR measurements was slightly smaller (inline-formula∼6.8 %) than that from the activation diameter (inline-formulaD₅₀) method due to the assumed internal mixing in the inline-formulaD₅₀ prediction. The inline-formulaN_CCN values predicted from bulk chemical composition of PMinline-formula₁ were higher (inline-formula∼11.5 %) than those from size-resolved composition measured by the AMS because a significant fraction of PMinline-formula₁ was composed of inorganic matter. The inline-formulaN_CCN values calculated from AMS measurement were underpredicted at 0.1 % and 0.2 % supersaturations, which could be due to underestimation of inline-formulaκ_org and overestimation of inline-formulaσ_s∕a. For SS values of 0.4 % and 0.7 %, slight overpredicted inline-formulaN_CCN values were found because of the internal mixing assumption. Our results highlight the need for accurately evaluating the effects of organics on both the hygroscopic parameter inline-formulaκ and the surface tension inline-formulaσ in order to accurately predict CCN activity.