Abstract. To investigate how atmospheric aerosol particles interact with chemical composition of cloud droplets, a ground-based counterflow virtual impactor (GCVI) coupled with a real-time single-particle aerosol mass spectrometer (SPAMS) was used to assess the chemical composition and mixing state of individual cloud residue particles in the Nanling Mountains (1690 m a.s.l.), southern China, in January 2016. The cloud residues were classified into nine particle types: aged elemental carbon (EC), potassium-rich (K-rich), amine, dust, Pb, Fe, organic carbon (OC), sodiumrich (Na-rich) and "Other". The largest fraction of the total cloud residues was the aged EC type (49.3 %), followed by the K-rich type (33.9 %). Abundant aged EC cloud residues that mixed internally with inorganic salts were found in air masses from northerly polluted areas. The number fraction (NF) of the K-rich cloud residues increased within southwesterly air masses from fire activities in Southeast Asia. When air masses changed from northerly polluted areas to southwesterly ocean and livestock areas, the amine particles increased from 0.2 to 15.1 % of the total cloud residues. The dust, Fe, Pb, Na-rich and OC particle types had a low contribution (0.5-4.1 %) to the total cloud residues. Higher fraction of nitrate (88-89 %) was found in the dust and Na-rich cloud residues relative to sulfate (41-42 %) and ammonium (15-23 %). Higher intensity of nitrate was found in the cloud residues relative to the ambient particles. Compared with nonactivated particles, nitrate intensity decreased in all cloud residues except for dust type. To our knowledge, this study is the first report on in situ observation of the chemical composition and mixing state of individual cloud residue particles in China.
We use a single‐particle aerosol mass spectrometer coupled with a ground‐based counterflow virtual impactor to measure the chemical compositions of individual submicron fog droplet residues. This is the first report on single particle mass spectrometry measurements of fog droplet residual particles at ground level in an urban area. We show that most of the fog droplet residues were composed of elemental carbon (EC) (67.7%), followed by K‐rich (19.2%) and mineral dust/metal (12.3%) particles. The predominance of EC‐containing particles demonstrated that these particles could be effective fog nuclei and highlights the important influence of anthropogenic emissions on regional climate system. Compared with interstitial and ambient aerosols, nitrate was enhanced, sulfate was depressed, and ammonium‐ and organics‐containing particles were hardly found in the fog droplet residues during fog events, suggesting that dust and metal particles containing nitrate may be preferentially activated and that ammonium and organics may not play important roles in fog formation in Guangzhou. We also present direct observational evidence that trimethylamine and hydroxymethanesulfonate are not found within fog droplet residues, although we previously observed enhanced gas‐to‐particle partitioning of these compounds by fog processing. Additionally, higher fraction or intensities of [K]+, [Fe]+, and [SiO3]− were found in fog droplet residues than in ambient and interstitial particles.
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