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. Hygroscopicity plays crucial roles in determining aerosol optical propertiesand aging processes in the atmosphere. We investigated submicron aerosolhygroscopicity and composition by connecting an aerosol time-of-flight massspectrometer (ATOFMS) in series to a hygroscopic tandem differentialmobility analyzer (HTDMA), to characterize hygroscopicity and composition ofambient aerosols in Shanghai, China. The HTDMA–ATOFMS data suggested thatparticle types, including biomass burning, elemental carbon (EC), dust/ash, organic particles,cooking particles and sea salt, were shown to have distinct hygroscopicitydistributions. Peak intensities in particle spectra were found to be nonlinearlycorrelated with hygroscopicity, and the correlations were variant withparticle types. Based on the measured hygroscopicity–composition relations,we developed a statistical method to estimate ambient particlehygroscopicity just from their mass spectra. The method was applied toanother ambient ATOFMS dataset sampled from 12 to 28 September 2012 in Shanghai. The estimated hygroscopicity suggested thatambient particles were present in three apparent hygroscopicity modes, whosegrowth factors peaked at 1.05, 1.42 and 1.60 (85 % relative humidity, RH). Theestimated growth factor (GF) were divided into four bins as , 1.1–1.3, 1.3–1.5and >1.5 to represent the nearly hydrophobic (NH),less-hygroscopic (LH), more-hygroscopic (MH) and sea salt (SS) modes. Numbercontributions of particle types to hygroscopicity modes showed consistentresults with the HTDMA–ATOFMS experiment. Based on the combined informationon particle composition, hygroscopicity, air mass back trajectories andambient pollutant concentrations, we inferred that the NH, LH, MH and SS modeswere characterized by primary organic aerosol (POA)  ∕  EC, secondary organic aerosol (SOA), secondary inorganic aerosol (SIA) and salt compositions, respectively.The proposed method would provide additional information to the study ofparticle mixing states, source identification and visibility variation.

Direct links between hygroscopicity and mixing state of ambient aerosols: estimating particle hygroscopicity from their single-particle mass spectra