Brown carbon (BrC) has been recognized as an important light-absorbing carbonaceous aerosol, yet understanding of its influence on regional climate and air quality has been lacking, mainly due to the ignorance of regional coupled meteorology-chemistry models. Besides, assumptions about its emissions in previous explorations might cause large uncertainties in estimates. Here, we implemented a BrC module into the WRF-Chem model that considers source-dependent absorption and avoids uncertainties caused by assumptions about emission intensities. To our best knowledge, we made the first effort to consider BrC in a regional coupled model. We then applied the developed model to explore the impacts of BrC absorption on radiative forcing, regional climate, and air quality in East Asia. We found notable increases in aerosol absorption optical depth (AAOD) in areas with high OC concentrations. The most intense forcing of BrC absorption occurs in autumn over Southeast Asia, and values could reach around 4 W m(-2). The intensified atmospheric absorption modified surface energy balance, resulting in subsequent declines in surface temperature, heat flux, boundary layer height, and turbulence exchanging rates. These changes in meteorological variables additionally modified near-surface dispersion and photochemical conditions, leading to changes of PM2.5 and O-3 concentrations. These findings indicate that BrC could exert important influence in specific regions and time periods. A more in-depth understanding could be achieved later with the developed model.
China experiences severe particulate matter (PM) pollution. Although a monitoring network for PM2.5 (diameter < 2.5 mu m) has been set up in more than 100 major Chinese cities, insufficient spatial coverage of observations limits the study of the temporal and spatial characteristics, influencing factors, and component of PM2.5. In this study, we conducted a one year air quality simulation using a regional climate-chemistry model and evaluated the simulation's performance based on in situ observations concerning meteorological elements and PM2.5 concentrations. The simulated results showed that, higher PM2.5 concentrations appeared in northern China and the Sichuan Basin, and the maximal value occurred in winter. Furthermore, Vertical PM2.5 concentrations presented a gradual decreasing trend from the surface, whereas in southern coastal cities the profiles were unsteady with a secondary peak in the lower layer. Meteorological conditions were conducive to both pollutant diffusion and removal in summer, whereas stagnant conditions appeared in winter, characterized by high sea level pressure (SLP), the lowest planetary boundary layer height (PBLH), and 2-m temperature (T2). In provincial capital cities, PM2.5 was positively correlated with residential emissions but negatively correlated with precipitation, 10-m wind speed, T2, PBLH, and industrial emissions. Finally, we utilized the simulation results to investigate the component variations of PM2.5. Results indicated that primary PM2.5 components had significantly higher concentrations in northern China where residential heating is the major source of PM2.5 emissions, whereas they had lower concentrations in southern China. Secondary components played a crucial role in PM2.5 mass in eastern China. This study provided a clear perspective of seasonal variations, horizontal and vertical distributions of PM2.5 and its components and influence factors, which could be used in subsequent studies to investigate the formation mechanism and emission sources of PM2.5.
The lockdowns implemented during the coronavirus disease 2019 (COVID-19) pandemic provide a unique opportunity to investigate the impact of emission sources and meteorological conditions on the trans-boundary transportation of black carbon (BC) aerosols to the Tibetan Plateau (TP). In this study, we conducted an integrative analysis, including in-situ observational data, reanalysis datasets, and numerical simulations, and found a significant reduction in the trans-boundary transport of BC to the TP during the 2020 pre-monsoon season as a result of the lockdowns and restrictive measures. Specifically, we observed a decrease of 0.0211 mu g m- 3 in surface BC concentration over the TP compared to the 2016 pre-monsoon period. Of this reduction, approximately 6.04 % can be attributed to the decrease in emissions during the COVID-19 pandemic, surpassing the 4.47 % decrease caused by changes in meteorological conditions. Additionally, the emission reductions have weakened the transboundary transport of South Asia BC to the TP by 0.0179 mu g m � 2s 1; indicating that the recurring spring atmospheric pollution from South Asia to the TP will be alleviated through the reduction of anthropogenic emissions. Moreover, it is important to note that BC deposition on glaciers contributes significantly to glacier melting due to its enrichment, posing a threat to the water sustainability of the TP. Therefore, urgent measures are needed to reduce emissions from adjacent regions to preserve the TP as the Asian Water Tower.
In this study, in situ observations were conducted for six criteria air pollutants (PM2.5, PM10, SO2, NO2, CO, and O-3) at 23 sites in western China for 1 year. Subsequently, the detailed Weather Research and Forecasting model coupled with Chemistry (WRF-Chem) results for the pollutants were determined. The WRF-Chem model provided a clear perspective on the spatiotemporal distribution of air pollutants. High pollutant concentrations were mainly observed over highly populated mega-city regions, such as Sichuan and Guanzhong basins, whereas low concentration levels were observed over the Tibetan Plateau (TP). The TP also showed an increased concentration of O-3. Seasonally, all six pollutants except O-3 exhibited high concentration values during winter and low values during summer. O-3 concentrations exhibited an opposite seasonal variation in low-altitude regions. Unlike other pollutants that exhibited gradually decreasing concentrations with an increase in altitude, O-3 concentrations revealed an increasing trend. Furthermore, NO2 concentrations gradually increased in the upper atmosphere possibly due to lighting and stratospheric transmission. Atmospheric pollution is closely related to emissions and meteorological variations in western China. Meteorological conditions in the summer are conducive to pollutant dispersion and wet scavenging; however, unfavourable weather conditions (high pressure as well as a low planetary boundary layer height and precipitation level) in the winter can further worsen air pollution. Atmospheric pollutants from various emission sectors generally exhibited varying monthly profiles. In six typical cities, pollutants were positively correlated with multiple emission sources except for industrial emissions. Further sensitivity simulations indicated that eliminating residential emissions resulted in the largest decrease (up to 70%) in PM2.5 and PM10 concentrations. The most significant reductions in the concentrations of SO2 and NO2 were achieved by eliminating industrial and transportation emissions, respectively. The outcomes of this study could be helpful for future studies on pollution formation mechanisms as well as environmental and health risk assessments in western China. (C) 2019 Elsevier Ltd. All rights reserved.
Black carbon (BC) as the main component of pollutants in the Arctic plays an important role on regional climate change. In this study, we applied the regional climate-chemistry model, WRF-Chem, to investigate the spatial distribution, transportation, and impact factors of BC in the Arctic. Compared with reanalysis data and observations, the WRF-Chem performed well in terms of the seasonal variations of meteorological parameters and BC concentrations, indicating the applicability of this model on Arctic BC simulation works. Our results showed that the BC concentrations in the Arctic had an obviously seasonalvariation pattern. Surface BC concentrations peaked during winter and spring seasons, while the minimum occurred during summer and autumn seasons. For the vertical distribution, BC aerosols mainly concentrated in the Arctic lower troposphere, and most of BC distributed near the surface during winter and spring seasons and in the higher altitude during other seasons. The seasonality of BC was associated with the seasonal change of meteorological field. During winter, the significant northward airflow prevailing in northern Eurasia caused the transport of accumulated pollutants from this region into the Arctic. The similar but weakened northward airflow pattern and the anticyclone activity during spring can allow pollutants to be transported to the Arctic lower troposphere. Moreover, the more stable atmosphere during winter and spring seasons made BC accumulated mainly near the surface. During summer and autumn seasons, the less stable boundary layer and the cyclone activity in the Arctic facilitated the diffusion of pollutants into the higher altitude. Meanwhile, the higher relative humidity can promote the wet removal process and lead to the relatively lower BC concentrations near the surface. Compared with the seasonal change of emission, our analysis showed that the seasonal variation of meteorological field was the main contributor for the seasonality of BC in the Arctic. (C) 2019 Elsevier Ltd. All rights reserved.
The formation mechanism of air pollution events in the Sichuan Basin (SB), which is the fourth most heavily polluted area in China, has not been fully revealed. This study investigated the formation mechanism of a severe air pollution event over the SB using synoptic approaches and model simulations. The results can be summarized as follows: (1) Heavy air pollution in the SB was characterized by low visibility, low atmospheric boundary layer (ABL) height, high temperature, high relative humidity, strong temperature inversion layer, subsidence in the troposphere, high water vapor content between 500 and 900 hPa, southerly winds in the low troposphere, and surface winds with low speed and irregular direction. (2) Air quality in the SB was closely related to the weather system at 700 hPa over the basin. When the 700 hPa weather system affecting the SB was a high-pressure system, the subsidence and stable atmospheric stratification increased the air pollutant concentrations near the ground. When the 700 hPa weather system affecting the SB was a low-pressure system and the basin was in front of this low-pressure system, southwesterly warm and moist airflow and adiabatic subsidence warming formed the thick temperature inversion layer over the basin. As a result, the temperature inversion layer trapped air pollutants in the basin and induced the heavy air pollution event. When the 700 hPa weather system over the SB was a low-pressure system and the basin was behind the low-pressure system, the dry and cold airflow from the north invaded southward to the basin and broke the temperature inversion layer. Consequently, air pollutants dispersed vertically, resulting in decreased concentrations near the ground. (3) Air pollutants from December 17, 2017 to January 4, 2018 were mainly from local emissions. (4) The WRF-Chem model not only reproduced the variations in PM2.5 concentrations, the ABL height, and the height-time cross-sections of temperature, water vapor content, and wind over Chengdu during the air pollution event, but also revealed the formation mechanism of this heavy air pollution event. The results of this study reveal the formation mechanism of winter heavy air pollution events over the SB and help develop effective regional air quality management strategies to reduce the likelihood of local air pollution events and minimize the adverse impacts of air pollution.
Seasonal open biomass burning contributes to significant carbonaceous aerosol loading over South Asia. This study analyzes long-term trends in emissions in two hot spot regions, Myanmar and Punjab, based on data from the Global Fire Emissions Database (GFED4s) and Fire INventory (FINN) from the National Center for Atmospheric Research (NCAR). Our analysis reveals that emissions during active fire seasons increase by approximately 83-106% and 2338-3054% for Punjab and Myanmar, respectively, compared to the estimates of anthropogenic emissions obtained with FINN. We also examine the impact of carbonaceous aerosol from open biomass burning on regional weather by using the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem) to conduct a year-long simulation of the post-monsoon and pre-monsoon periods when active fires were reported. The results indicate that the carbonaceous aerosol is vertically lofted by as much as 3-5 km into the atmosphere and, rising as high as the 850 hPa level from the surface, disperses horizontally throughout South Asia. Our calculations on the radiative forcing suggest that changes of up to -6.14 W m(-2) and -0.50 W m(-2), and -42.76 W m(-2) and -1.91 W m(-2) occur at the surface and at the top of the atmosphere over Punjab and Myanmar, respectively. We also find that carbonaceous aerosol (black carbon + organic carbon), similar to black carbon (BC), reduces the surface temperature, despite the scattering effects of organic carbon (OC). Overall, open biomass burning causes the surface temperature to decrease by 2 K, the relative humidity to increase by 8% and the planetary boundary layer height to change by as much as 600 m. Changes in the precipitation patterns and volume due to the carbonaceous aerosol from open biomass burning, however, are negligible when considering only the direct radiative feedback.
Black carbon (BC) exerts a potential influence on climate, especially in the Arctic, where the environment is very sensitive to climate change. Therefore, the study of climate effects of BC in this region is particularly important. In this study, numerical simulations were performed using the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem) in the Arctic in winter and spring for two years to investigate the atmospheric BC causing changes in surface radiation, meteorology, and atmospheric stability. Generally, WRF-Chem well reproduced the temporal variations of meteorological variables and BC concentration. Numerical simulations showed that BC concentrations in the Arctic in winter were mostly higher than those in spring, and the BC-induced near-surface temperature changes were also stronger. The effects of BC on near-surface water vapor mixing ratio were consistent with the spatial pattern of near-surface temperature changes. That was probably the result of the regional circulation anomaly due to the temperature changes. Additionally, the distributions of near-surface temperature changes and horizontal wind changes also reflected in the distribution of planetary boundary layer height. Ultimately, this study revealed that the downward longwave radiation related to cloudiness changes played an important role for driving near-surface temperature in the Arctic in winter. While in spring, the relatively less changes in near-surface temperature may be the result of the mutual compensation between the surface longwave and shortwave radiation effects. (C) 2020 Elsevier B.V. All rights reserved.
Changes in snow albedo (SA) on the Limari, Choapa, Aconcagua and Maipo basins of the Central Andes of Chile (CAC) are associated with the possible deposition of light-absorbing particles in the austral spring. We correlate SA with daily data of snow cover, aerosol optical depth (AOD) and land surface temperature (LST) available from the Moderate Resolution Imaging Spectroradiometer (MODIS) onboard the NASA Terra satellite between 2000 and 2016, and other derived parameters such as days after albedo (DAS) and snow precipitation (SP). We used satellite pixels with 100% snow cover to obtain monthly average value of SA, LST, AOD, DAS and SP from September to November performing multiple regression analysis. We show that in Maipo, after considering LST, AOD represents an important role in changes induced to SA. The multiple regression model illustrates that AOD increases can reduce the SA during spring months by 13.59, 0.01, 0.77 and 3.8% in Limari, Choapa, Aconcagua and Maipo, respectively. In addition, we used a numerical prediction Weather Research and Forecasting model coupled with Chemistry (WRF-Chem), showing that the black carbon distribution and average daily AOD are associated with the SA decrease of 0.15 in the Maipo basin between September 29 and 30, 2016. The WRF-Chem output showed aerosols are transported mainly with dominating westerly winds to the Limari and Maipo basins. Our results further suggest that SA decrease due to AOD may be originated in the largest industrial and urban areas in Chile, producing a negative impact on the hydrological resource, generated in the CAC.
Residential sector emissions of aerosols, primarily from solid fuels burned for cooking and heating purposes, are high in black carbon, a component that absorbs radiation efficiently across a wideband of wavelengths. Mitigation of residential sector emissions has been suggested as a method to rapidly reduce anthropogenic global warming. This study presents model results from a regional model with coupled chemistry, aerosols, and dynamics over an East Asian domain for January 2014 to investigate the radiative effects of residential sector emissions. Model results are evaluated against surface measurements of particulate matter and remote sensing products, comparing well but with a high aerosol optical depth bias over Sichuan and low single scattering albedo over many locations. We calculate effective radiative forcing of residential sector aerosols at the top of the atmosphere of +1.22W/m(2) over Eastern China, +1.04W/m(2) due to shortwave and +0.18W/m(2) due to longwave forcing. We decompose the shortwave forcing into component parts and find the direct radiative effect is the dominant component (+0.79W/m(2)), with a smaller contribution from semidirect effects (+0.54W/m(2)) partly countered by negative indirect effects (-0.29W/m(2)). The effective radiative forcing varies from 0.20 to 1.97W/m(2) across a reasonable range of black carbon to total carbon emission ratios for the residential sector. Overall, this study shows that mitigation of the residential sector is likely a viable method to locally reduce short-term atmospheric warming in China, but efforts are needed to reduce uncertainty in composition of residential sector emissions to be confident in this conclusion.