Nitrogen-containing organic compounds (NOCs) may potentially contribute to aqueous secondary organic aerosols, yet the different formation of NOCs in aerosol particles and cloud droplets remains unclear. With the in-situ measurements performed at a mountain site (1690 m a.s.l.) in southern China, we investigated the formation of NOCs in the cloud droplets and the cloud-free particles, based on their mixing state information of NOCs-containing particles by single particle mass spectrometry. The relative abundance of NOCs in the cloud-free particles was significantly higher than those in cloud residual (cloud RES) particles. NOCs were highly correlated with carbonyl compounds (including glyoxalate and methylglyoxal) in the cloud-free particles, however, limited correlation was observed for cloud RES particles. Analysis of their mixing state and temporal variations highlights that NOCs was mainly formed from the carbonyl compounds and ammonium in the cloud-free particles, rather than in the cloud RES particles. The results support that the formation of NOCs from carbonyl compounds is facilitated in concentrated solutions in wet aerosols, rather than cloud droplets. In addition, we have identified the transport of biomass burning particles that facilitate the formation of NOCs, and that the observed NOCs is most likely contributed to the light absorption. These findings have implications for the evaluation of NOCs formation and their contribution to light absorption.

A single particle aerosol mass spectrometry (SPAMS) was deployed to investigate the mixing state and chemical processing of Pb-rich particles in suburban Beijing. Based on a large dataset of mass spectra, Pb-rich particles were classified into Pb-O-Cl-N-S (55%), Pb-N (17%), Pb-N-S (15%), and Pb-EC (7%). Residual coal combustion, industrial activities, and meteorological conditions were identified as main factors regulating the variations of Pb-rich particles in the atmosphere. The highest abundance of the Pb-rich particles was observed during heating period (HP) primarily due to the increase in coal usage. Pb in Pb-O-Cl-N-S type was identified in forms of PbO, PbCl2, and Pb(NO3)2. Dominantly presented in the form of Pb(NO3)2, Pb-N type represented the completely transformed Pb-rich particles from PbO/PbCl2 by atmospheric processes. It is found that PbCl2 and PbO could be transformed to Pb(NO3)2, highly dependent on the amount of NO2 and RH. Significant enhancement of nitrate in Pb-O-Cl-N-S particles was observed when the RH was greater than 60%, emphasizing the importance of heterogeneous hydrolysis of N2O5 on the formation of Pb(NO3)2. Compared with non-carcinogenic PbCl2/PbO and insoluble PbO, soluble and carcinogenic Pb(NO3)2 produced by atmospheric processes may significantly enhance negative effects of Pb-rich particles on human health and the ecosystem.

To investigate the composition and possible sources of particles, especially during heavy haze pollution, a single particle aerosol mass spectrometer (SPAMS) was deployed to measure the changes of single particle species and sizes during October of 2014, in Beijing. A total of 2,871,431 particles with both positive and negative spectra were collected and characterized in combination with the adaptive resonance theory neural network algorithm (ART-2a). Eight types of particles were classified: dust particles (dust, 8.1%), elemental carbon (EC, 29.0%), organic carbon (OC, 18.0%), EC and OC combined particles (ECOC, 9.5%), Na-K containing particles (NaK, 7.9%), K-containing particles (K, 21.8%), organic nitrogen and potassium containing particles (KCN, 2.3%), and metal-containing particles (metal, 3.6%). Three haze pollution events (P1, P2, P3) and one clean period (clean) were analyzed, based on the mass and number concentration of PM2.5 and the back trajectory results from the hybrid single particle Lagrangian integrated trajectory model (Hysplit-4 model). Results showed that EC, OC and K were the major components of single particles during the three haze pollution periods, which showed clearly increased ratios compared with those in the clean period. Results from the mixing state of secondary species of different types of particles showed that sulfate and nitrate were more readily mixed with carbon-containing particles during haze pollution episodes than in clean periods.

There is a large uncertainty in evaluating the radiative forcing from aerosol-radiation and aerosol-cloud interactions due to the limited knowledge on aerosol properties. In-situ measurements of aerosol physical and chemical properties were carried out in 2012 at Mt. Huang (the Yellow Mountain), a continental background mountainous site in eastern China. An aerosol optical closure study was performed to verify the model outputs by using the measured aerosol optical properties, in which a spherical Mie model with assumptions of external and core-shell mixtures on the basis of a two-component optical aerosol model and high size-segregated element carbon (EC) ratio was applied. Although the spherical Mie model would underestimate the real scattering with increasing particle diameters, excellent agreement between the calculated and measured values was achieved with correlation coefficients above 0.98. Sensitivity experiments showed that the EC ratio had a negligible effect on the calculated scattering coefficient, but largely influenced the calculated absorption coefficient. The high size-segregated EC ratio averaged over the study period in the closure was enough to reconstruct the aerosol absorption coefficient in the Mie model, indicating EC size resolution was more important than time resolution in retrieving the absorption coefficient in the model. The uncertainties of calculated scattering and absorption coefficients due to the uncertainties of measurements and model assumptions yielded by a Monte Carlo simulation were ±6% and ±14% for external mixture and ±9% and ±31% for core-shell mixture, respectively. This study provided an insight into the inherent relationship between aerosol optical properties and physicochemical characteristics in eastern China, which could supplement the database of aerosol optical properties for background sites in eastern China and provide a method for regions with similar climate.