Primary nature of brown carbon absorption in a frigid atmosphere with strong haze chemistry.

Severe haze hovered over Harbin during the heating season of 2019-2020, making it one of the ten most polluted Chinese cities in January of 2020. Here we focused on the optical properties and sources of brown carbon (BrC) during the extreme atmospheric pollution periods. Enhanced formation of secondary BrC (BrCsec) was evident as relative humidity (RH) became higher, accompanied with a decrease of ozone but concurrent increases of aerosol water content and secondary inorganic aerosols. These features were generally similar to the characteristics of haze chemistry observed during winter haze events in the North China Plain, and indicated that heterogeneous reactions involving aerosol water might be at play in the formation of BrCsec, despite the low temperatures in Harbin. Although BrCsec accounted for a substantial fraction of brown carbon mass, its contribution to BrC absorption was much smaller (6 vs. 28%), pointing to a lower mass absorption efficiency (MAE) of BrCsec compared to primary BrC. In addition, emissions of biomass burning BrC (BrCBB) were inferred to increase with increasing RH, coinciding with a large drop of temperature. Since both the less absorbing BrCsec and the more absorbing BrCBB increased as RH became higher, the MAE of total BrC were largely unchanged throughout the measurement period. This study unfolded the contrast in the source apportionment results of BrC mass and absorption, and could have implications for the simulation of radiative forcing by brown carbon.

[Numerical modeling analysis of secondary organic aerosol (SOA) combined with the ground-based measurements in the Pearl River Delta region].

Two simulations were conducted with different secondary organic aerosol (SOA) methods-VBS (volatile basis set) approach and SORGAM (secondary organic aerosol model) , which have been coupled in the WRF/Chem (weather research and forecasting model with chemistry) model. Ground-based observation data from 18th to 25th November 2008 were used to examine the model performance of SOA in the Pearl River Delta(PRD)region. The results showed that VBS approach could better reproduce the temporal variation and magnitude of SOA compared with SORGAM, and the mean absolute deviation and correlation coefficient between the observed and the simulated data using VBS approach were -4.88 microg m-3 and 0.91, respectively, while they were -5.32 microg.m-3 and 0. 18 with SORGAM. This is mainly because the VBS approach considers SOA precursors with a wider volatility range and the process of chemical aging in SOA formation. Spatiotemporal distribution of SOA in the PRD from the VBS simulation was also analyzed. The results indicated that the SOA has a significant diurnal variation, and the maximal SOA concentration occurred at noon and in the early afternoon. Because of the transport and the considerable spatial distribution of O3 , the SOA concentrations were different in different PRD cities, and the highest concentration of SOA was observed in the downwind area, including Zhongshan, Zhuhai and Jiangmen.

[Application of on-line single particle aerosol mass spectrometry (SPAMS) for studying major components in fine particulate matter].

Based on preliminary studies by aerosol time-of-flight mass spectrometer (ATOFMS) and single particle aerosol mass spectrometer (SPAMS), typical methods for identifying the number of particles (or particle count) for five major components including sulfate, nitrate, ammonium, organic carbon (OC), and elemental carbon (EC) in China and abroad were summarized. In this study, combined with the characteristics of single particle mass spectrum by SPAMS, an optimized method is proposed. With field measurement using SPAMS during January 2013 in Beijing, particle counts of sulfate, nitrate, ammonium, OC, and EC determined by different methods were compared. The comparison with results of off-line filter analyses for these five components proved that the method proposed in this study is comparable and optimized. We also suggest factors needed to be considered in future application of SPAMS and other areas that require in-depth research.

[Research progress and direction of atmospheric brown carbon].

Organic aerosol is one of the most important components of atmospheric aerosols. In recent years, organic aerosol has been found and proved to be light absorbing in UV-Visible region. Light absorbing organic carbon (also named as brown carbon) has been one of the forefronts in the field of atmospheric research. Its light absorption contributions to radiative forcing, regional air quality, and global climate change have drawn much attention. Regional air pollution is complex in China. Frequent visibility decline and severe regional haze episodes occurred since January 2013. Previous studies showed high amount of estimated columnar light-absorbing organic carbon in China, and according to current research findings, major sources of fine particulate matter in China (e. g. biomass burning and fossil fuel combustion) were also recognized as the main sources for brown carbon. Considering the high abundance of brown carbon in atmosphere, there is a great need to reconsider and reevaluate contributions of organic aerosol to light absorption, especially its role in haze formation and radiative forcing. However, up to now, basic researches on light absorbing organic carbon are still limited in China. This study aimed to elucidate the need for basic research on brown carbon, summarize previous studies and research progress from different aspects such as sources, composition, measurement, mass concentration distribution, optical property, radiative forcing of brown carbon, point out the existing problems and deficiencies, and put forward suggestions for future study.

[Improvement and application of the method for determination of OCEC split].

Aerosol samples were collected in Beijing (BD) and Atlanta (GT) from July to August in 2011 using a Micro-Orifice Uniform Deposit Impactor (MOUDI) (0.18-18 microm, eight-stage) for organic carbon (OC) and elemental carbon (EC) measurement (Sunset Laboratory Inc, USA). The laser intensity of blank filters decreased with temperature in the process of OC & EC analysis because the structure of quartz filters was changed when burned which largely affected the determination of low concentration samples' splits. It would increase the accuracy of OC & EC split to determine it manually after the change of blank filter's laser intensity was recouped. The concentrations and size distributions of OC & EC using the improved method were different from taking the moment when oxygen was introduced as the split. The split may appear before oxygen addition, when the sample was rich in metal or substances that can be decomposed after heated. The concentrations of carbonaceous components were higher at BD than those at GT. The size distributions of OC showed a bimodal pattern with peaks appeared in the particles with size of (0.56-1.0) microm and (3.2-5.6) microm. The peak concentrations of OC were (2.82 +/- 1.59) microg x m(-3) and (1.95 +/- 0.76) microg x m(-3) at BD, and (1.28 +/- 0.41) microg x m(-3) and (0.64 +/- 0.19) microg x m(-3) at GT. EC showed a bimodal pattern at BD with peaks in particles with size of (0.56-1.0) microm and (3.2-5.6) microm, while showed a trimodal pattern at GT. The peak concentrations at BD were (0.32 +/- 0.24) microg x m(-3) and (0.26 +/- 0.19) microg x m(-3). EC at GT was preferably enriched in particles with size of (0.18-0.56) microm, the mass concentrations of EC in this size accounted for 44.6%. The OC and EC were more concentrated in accumulation mode at GT than those at BD, the reason may be that the main pollution source of GT is motor vehicle emission, while there are more industrial gas emissions at BD.