Spatial distribution, sources, and direct radiative effect of carbonaceous aerosol along a transect from the Arctic Ocean to Antarctica.

Carbonaceous aerosols (CA) have a high impact on air quality and climate. However, the composition and spatial variability of CA in the marine boundary layer (MBL) remain understudied, especially in the remote regions. Here, atmospheric organic carbon (OC) and elemental carbon (EC) measurements using DRI Model 2001 Thermal/Optical Carbon Analyzer in the MBL were performed during the Chinese Antarctic (2019-2020) and Arctic (2021) research expedition, spanning about 160 latitudes. Due to varying intensities of atmospheric transport from the continents, a significant latitudinal gradient in OC and EC was observed. OC exhibited the highest concentration over the coastal East Asia (CEA), with a mean of 4324 ng m-3 (358-18027 ng m-3), followed by the Arctic Ocean (AO). Similar OC levels were detected over the Southern Ocean (SO) and the Antarctic Ice Sheet (AIS). Similarly, the highest EC was also observed over CEA, with a mean of 867 ng m-3 (71-3410 ng m-3), followed by AO and SO, while the lowest EC appeared over the AIS, with a mean of 30 ng m-3 (2-70 ng m-3). The lower Char-EC/Soot-EC ratios over AO and CEA compared to SO and AIS indicated that fossil fuel combustion contributed more to EC over AO and CEA, while biomass burning played a more significant role in EC levels over SO and AIS. The high OC/EC ratio over AIS was associated with an extremely low EC level and the formation of secondary OC over AIS. SBDART model results suggested that EC had a net warming effect on the atmospheric column, with the highest direct radiative effects (DRE) over AO (5.50 ± 0.15 W m-2, corresponding a heating rate of 0.15 K day-1) and the lowest DRE over SO (1.35 ± 0.04 W m-2, corresponding a heating rate of 0.04 K day-1).

Impacts of springtime biomass burning in Southeast Asia on atmospheric carbonaceous components over the Beibu Gulf in China: Insights from aircraft observations.

Limited by the scarcity of in situ vertical observation data, the influences of biomass burning in Southeast Asia on major atmospheric carbonaceous compositions in downwind regions have not been thoroughly studied. In this study, aircraft observations were performed to obtain high time-resolved in situ vertical distributions of black carbon (BC) as well as carbon monoxide (CO) and carbon dioxide (CO2). Four types of profiles were revealed: Mode I (from 2000 to 3000 m, the BC, CO and CO2 concentrations were enhanced), Mode II (with increasing altitude, the BC, CO and CO2 concentrations almost decreased), Mode III (inhomogeneous vertical BC, CO and CO2 profiles with BC peaks were observed from 2500 to 3000 m) and Mode IV (the BC, CO and CO2 concentrations increased above 1500 m). Furthermore, simulations were conducted to calculate radiative forcing (RF) caused by BC and study the heating rate (HR) of BC in combination with the vertical BC profiles. A larger BC distribution in the atmosphere resulted in a sharp RF change from negative to positive values, imposing a nonnegligible influence on the atmospheric temperature profile, with maximum HR values ranging from 0.4 to 5.8 K/day. The values of the absorption Ångström exponent (AAE) were 1.46 ± 0.11 and 1.48 ± 0.17 at altitudes from 1000 to 2000 and 2000-3000 m, respectively. The average BC light absorption coefficient at the 370 nm wavelength (α BC (370)) accounted for 50.3 %-76.8 % of the α (370), while the brown carbon (BrC) light absorption coefficient at the 370 nm wavelength (α BrC (370)) contributed 23.2 %-49.7 % to the α (370) at altitudes of 1000-2000 m. At altitudes of 2000-3000 m, α BC (370) and α BrC (370) contributed 43.8 %-88.2 % and 11.8 %-56.2 % to the α (370), respectively. These findings show that calculations that consider the surface BC concentration but ignore the vertical BC distribution could result in massive uncertainties in estimating the RF and HR caused by BC. This study helped achieve a deeper understanding of the influences of biomass burning over the region of Southeast Asia on the profiles of atmospheric carbonaceous compositions and atmospheric BC absorption and its warming effect.

The feedback effects of aerosols from different sources on the urban boundary layer in Beijing China.

The interaction of aerosols and the planetary boundary layer (PBL) plays an important role in deteriorating urban air quality. Aerosols from different sources may have different effects on regulating PBL structures owing to their distinctive dominant compositions and vertical distributions. To characterize the complex feedback of aerosols on PBL over the Beijing megacity, multiple approaches, including in situ observations in the autumn and winter of 2016-2019, backward trajectory clusters, and large-eddy simulations, were adopted. The results revealed notable distinctions in aerosol properties, vertical distributions and thermal stratifications among three types of air masses from the West Siberian Plain (Type-1), Central Siberian Plateau (Type-2) and Mongolian Plateau (Type-3). Low loadings of 0.28 ± 0.26 and 0.15 ± 0.08 of aerosol optical depth (AOD) appeared in the Type-1 and Type-2, accompanied by cool and less stable stratification, with a large part (80%) of aerosols concentrated below 1500 m. For Type-3, the AOD and single scattering albedo (SSA) were as high as 0.75 ± 0.54 and 0.91 ± 0.05, demonstrating severe pollution levels of abundant scattering aerosols. Eighty percent of the aerosols were constrained within a lower height of 1150 m owing to the warmer and more stable environment. Large-eddy simulations revealed that aerosols consistently suppressed the daytime convective boundary layer regardless of their origins, with the PBL height (PBLH) decreasing from 1120 m (Type-1), 1160 m (Type-2) and 820 m (Type-3) in the ideal clean scenarios to 980 m, 1100 m and 600 m, respectively, under polluted conditions. Therefore, the promotion of absorbing aerosols below the residual layer on PBL could be greatly hindered by the suppression effects generated by both absorbing aerosols in the upper temperature inversion layer and scattering aerosols. Moreover, the results indicated the possible complexities of aerosol-PBL interactions under future emission-reduction scenarios and in other urban regions.

Vertical evolution of black and brown carbon during pollution events over North China Plain.

The vertical distribution of carbonaceous aerosol impacts climate change, air quality and human health, but there is a lack of in-situ vertical observations of black (BC) and brown carbon (BrC). Thus, the characteristic of vertical profiles of BC concentration, particle number concentration (PNC), O3 concentration and optical absorption of BC and BrC were observed in a suburban site over North China Plain, where heavy pollution of PM2.5 and O3 always occurred in winter and summer, respectively. In winter, during a heavy pollution episode, the BC and PNC was near uniformly distributed within mixing layer (ML) (15.2 ± 6.7 µg m-3 and 678 ± 227 p cm-3, respectively) and decreased with altitude above the ML. The BC heating rate reached about 0.13 K h-1 during the heaviest pollution day. In summer, the BC concentration (2.9 ± 1.3 µg m-3) in ML during the middle O3 pollution events was higher than that (1.7 ± 0.6 µg m-3) during the light O3 pollution. The light absorption coefficients of BC at 880 nm and BrC at 375 nm measured in the early morning were lower than that in the daytime, and the contribution of BrC to total light absorption of carbonaceous aerosols was in the range of 27-47%. In addition, BC was effectively transported to high altitude than BrC in the daytime. The light absorption of secondary BrC in the daytime was higher 10-20% than that in the early morning. Simultaneously, the contribution of secondary BrC to the total BrC light absorption at 375 nm was range from 32% to 68% within 1000 m.

The formation mechanism of air pollution episodes in Beijing city: Insights into the measured feedback between aerosol radiative forcing and the atmospheric boundary layer stability.

Based on the high-resolution observation of meteorological factors profiles, particulate matter concentration and aerosol radiative forcing (ARF) from 25 August to 17 November 2018 in Beijing, the feedback between ARF and the atmospheric boundary layer (ABL) stability was systematically investigated during air pollution episodes. There was the initial explosive growth in particulate matter (PM) concentration that PM2.5 sharply increased from ~8µgm-3 to ~100µgm-3, with aerosol optical depth (AOD) increasing from ~0.25 to ~0.58. This was the transport phase dominated by the southerly winds. As PM increased, the high aerosol loading scattered more solar radiation cooling the earth-atmosphere system (ARF at the top of the atmospheric column (TOA): from ~5Wm-2 to ~-52Wm-2). Meanwhile, high aerosol loading absorbed more solar radiation and heated the atmospheric layer with ARF at the interior of the atmospheric column (ATM) increasing from ~21Wm-2 to ~42Wm-2. The absorption and scattering effects of aerosol together cooled the surface (ARF at the surface of the atmospheric column (SFC): from ~-16Wm-2 to ~-90Wm-2). Thus, the ABL stability rapidly increased in the following cumulative phase and heavy pollution phase with a strong temperature inversion (inversion depth of ~300-1000m) occurring. In turn, the persistent temperature inversion caused the significant accumulation of moisture (water vapor density of ~5-10gm-3) and pollutants, and PM were prone to physicochemical reactions in the high-humidity environment, further increasing PM. It was the constant feedback effect between ARF and the ABL stability that continually reduced atmospheric environmental capacity and aggravated air pollution (PM2.5 and AOD reaching ~95-125µgm-3 and ~1.38-1.75, respectively). Finally, the feedback was broken by dry, clean and strong north winds appearing in Beijing in the dissipation phase.