Air quality in Beijing has been improved significantly in recent years; however, our knowledge of the vertically resolved aerosol chemistry in summer remains poor. Here, we carried out comprehensive measurements of aerosol composition, gaseous species, and aerosol optical properties on a meteorological tower in Beijing in summer and compared with those measured in winter. Our results showed that aerosol liquid water (ALW) contributing approximately 50% of the total mass with higher values aloft played a crucial role in aerosol formation. Particularly, the higher nitrate concentration in city aloft than at the ground level during daytime was mainly due to the enhanced gas–particle partitioning driven by ALW and particle acidity. The vertical profiles of organic aerosol (OA) factors varied more differently in the urban boundary layer. Although the ubiquitous decreases in primary OA with the increase in height were mainly due to the influences of local emissions and vertical convection, the vertical differences in oxygenated OA between summer and winter may be related to the photochemical processing of different biogenic and anthropogenic volatile organic compounds. The single-scattering albedo, brown carbon, and absorption Ångstrom exponent of aerosol particles also presented different vertical profiles between day and night due to the vertical changes in aerosol chemistry.

Photochemical aging is a key atmospheric processing, yet the changes in physicochemical properties of organic aerosol (OA) during photochemical aging of primary emissions from cooking and burning are less understood. Here we conducted 12 burning (straw, wood, and coal) and cooking experiments to characterize the evolution of size distributions, volatility, and glass transition temperature (Tg) from fresh smoke to aged OA with an equivalent photochemical age of ∼1.5 days using an oxidation flow reactor‐thermodenuder‐aerosol mass spectrometer system. The mass spectra of OA showed significant changes during photochemical aging, for example, the rapid degradation of m/z 60 for straw and wood burning OA, and the large increase in f44 (fraction of m/z 44 in OA) for all OA. The contributions of non‐volatile compounds to the total OA in aged burning OA (1.6%–5.3%) decreased considerably compared with those in fresh burning smoke (2.3%–17.1%), suggesting that photochemical aging of primary emissions for ∼1.5 days produced more volatile secondary OA (SOA). Consistently, the pronounced formation of SOA below 150 nm was observed, and it showed more volatile properties than aged large particles. The Tg of OA under dry conditions (Tg,org) was estimated based on volatility distributions, and the results showed increased Tg,org during photochemical aging of biomass burning and coal combustion emissions, while decreased Tg,org for aged cooking OA. Overall, our results illustrate the different changes in size distributions, volatility, and Tg,org through photochemical aging of different primary emissions, which in turn affect their impacts on radiative forcing and human health.

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