Isotopic constraints on the atmospheric sources and formation of nitrogenous species in clouds influenced by biomass burning

Abstract. Predicting tropospheric cloud formation and subsequent nutrient deposition relies on understanding the sources and processes affecting aerosol constituents of the atmosphere that are preserved in cloud water. However, this challenge is difficult to address quantitatively based on the sole use of bulk chemical properties. Nitrogenous aerosols, mainly ammonium (NH4+) and nitrate (NO3-), play a particularly important role in tropospheric cloud formation. While dry and wet (mainly rainfall) deposition of NH4+ and NO3- are regularly assessed, cloud water deposition is often underappreciated. Here we collected cloud water samples at the summit of Mt. Tai (1545 m above sea level) in eastern China during a long-lasting biomass burning (BB) event and simultaneously measured for the first time the isotopic compositions (mean ±1σ) of cloud water nitrogen species (δ15N-NH4+ = −6.53 ‰ ± 4.96 ‰, δ15N-NO3- = −2.35 ‰ ± 2.00 ‰, δ18O-NO3- = 57.80 ‰ ± 4.23 ‰), allowing insights into their sources and potential transformation mechanism within the clouds. Large contributions of BB to the cloud water NH4+ (32.9 % ± 4.6 %) and NO3- (28.2 % ± 2.7 %) inventories were confirmed through a Bayesian isotopic mixing model, coupled with our newly developed computational quantum chemistry module. Despite an overall reduction in total anthropogenic NOx emission due to effective emission control actions and stricter emission standards for vehicles, the observed cloud δ15N-NO3- values suggest that NOx emissions from transportation may have exceeded emissions from coal combustion. δ18O-NO3- values imply that the reaction of OH with NO2 is the dominant pathway of NO3- formation (57 % ± 11 %), yet the contribution of heterogeneous hydrolysis of dinitrogen pentoxide was almost as important (43 % ± 11 %). Although the limited sample set used here results in a relatively large uncertainty with regards to the origin of cloud-associated nitrogen deposition, the high concentrations of inorganic nitrogen imply that clouds represent an important source of nitrogen, especially for nitrogen-limited ecosystems in remote areas. Further simultaneous and long-term sampling of aerosol, rainfall, and cloud water is vital for understanding the anthropogenic influence on nitrogen deposition in the study region.

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Isotopic Constraints on the Atmospheric Sources and Formation of Nitrogenous Species in Biomass-Burning-Influenced Clouds

10.5194/acp-2018-1196 ◽

2018 ◽

Author(s):

Yunhua Chang ◽

Yanlin Zhang ◽

Jiarong Li ◽

Chongguo Tian ◽

Linlin Song ◽

...

Keyword(s):

Biomass Burning ◽

Eastern China ◽

Chemical Properties ◽

Cloud Formation ◽

Transformation Mechanism ◽

Dinitrogen Pentoxide ◽

Computational Quantum Chemistry ◽

Bulk Chemical ◽

Isotopic Mixing ◽

First Time

Abstract. The interpretation of tropospheric cloud formation rests on understanding the sources and processes affecting aerosol constituents of the atmosphere that are preserved in cloudwater. However, this challenge is difficult to be quantitatively addressed based on the sole use of bulk chemical properties. Nitrogenous aerosols, mainly ammonium (NH4+) and nitrate (NO3−), play an important role in tropospheric cloud formation. Here we collected cloudwater samples at the summit of Mt. Tai (1545 m above sea level) in Eastern China during a long-lasting biomass burning (BB) event, and measured for the first time the isotopic compositions (mean ± 1σ) of cloudwater nitrogen species (δ15N-NH4+ = −6.53 ± 4.96 ‰, δ15N-NO3− = −2.35 ± 2.00 ‰, δ18O-NO3− = 57.80 ± 4.23 ‰), allowing insights into their sources and potential transformation mechanism within the clouds. Large contributions of BB to the cloudwater NH4+ (32.9 ± 4.6 %) and NO3− (28.2 ± 2.7 %) inventories were confirmed through a Bayesian isotopic mixing model, coupled with our newly-developed computational quantum chemistry module. Despite an overall reduction in total anthropogenic NOx emission due to effective emission control actions and stricter emission standards for vehicles, the observed cloud δ15N-NO3− values suggest that NOx emissions from transportation may have exceeded emissions from coal combustion. δ18O-NO3− values imply that the reaction of OH with NO2 is the dominant pathway of NO3− formation (57 ± 11 %), yet the contribution of heterogeneous hydrolysis of dinitrogen pentoxide was almost as important (43 ± 11 %).

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Wet Inorganic Nitrogen Deposition at the Daheitin Reservoir in North China: Temporal Variation, Sources, and Biomass Burning Influences

Atmosphere ◽

10.3390/atmos11111260 ◽

2020 ◽

Vol 11 (11) ◽

pp. 1260

Author(s):

Leixiang Wu ◽

Xiaobo Liu ◽

Kun Li ◽

Wanyun Xu ◽

Wei Huang ◽

...

Keyword(s):

Nitrogen Deposition ◽

Biomass Burning ◽

Wet Deposition ◽

North China ◽

Inorganic Nitrogen ◽

Chemical Properties ◽

Northern China ◽

N Deposition ◽

Rural Site ◽

Wet Season

Atmospheric nitrogen deposition is of great concern to both air quality and the ecosystem, particularly in northern China, which covers one-quarter of China’s cultivated land and has many heavily air polluted cities. To understand the characteristics of wet N deposition at rural sites in northern China, one-year wet deposition samples were collected in the Daheitin reservoir region. Due to the intense emissions of gaseous nitrogen compounds from heating activities during cold seasons and distinct dilution effects under different rainfall intensities and frequencies, the volume weighted mean concentrations of wet N deposition showed higher levels in dry seasons but lower levels in wet seasons. In contrast, the wet N deposition rates varied consistently with precipitation, i.e., high during the wet season and lower during the dry season. The annual wet deposition rate of total inorganic ions (the sum of NO3−–N and NH4+–N) at the rural site in North China from July 2019 to June 2020 was observed at 18.9 kg N ha−1 yr−1, still remained at a relatively high level. In addition, biomass burning activities are ubiquitous in China, especially in northern China; however, studies on its impact on wet N deposition are limited. Non-sea salt potassium ion (nss-K+) was employed as a molecular tracer to investigate the characteristics of biomass burning activities as well as their impact on the chemical properties of wet N deposition. Three precipitation events with high nss-K+ levels were captured during the harvest season (June to July). The variations in the patterns of nss-K+, deposited N species, and ratios of nss-K+ to nitrogen species as well as their relationships all indicated that biomass burning emissions contributed remarkably to NO3−–N but had a minor influence on NH4+–N.

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Total organic carbon and contribution from speciated organics in cloud water: Airborne data analysis from the CAMP<sup>2</sup>Ex field campaign

10.5194/acp-2021-403 ◽

2021 ◽

Author(s):

Connor Stahl ◽

Ewan Crosbie ◽

Paola Angela Bañaga ◽

Grace Betito ◽

Rachel A. Braun ◽

...

Keyword(s):

Organic Carbon ◽

Total Organic Carbon ◽

Biomass Burning ◽

Dicarboxylic Acids ◽

Cloud Water ◽

Water Soluble ◽

Monocarboxylic Acids ◽

Study Region ◽

Carbon Mass ◽

Measured Mass

Abstract. This work focuses on total organic carbon (TOC) and contributing species in cloud water over Southeast Asia using a rare airborne dataset collected during NASA’s Cloud, Aerosol and Monsoon Processes Philippines Experiment (CAMP2Ex), in which a wide variety of maritime clouds were studied, including cumulus congestus, altocumulus, altostratus, and cumulus. Knowledge of TOC levels and their contributing species is needed for improved modeling of cloud processing of organics and to understand how aerosols and gases impact and are impacted by clouds. This work relies on 159 samples collected with an Axial Cyclone Cloud water Collector at altitudes of 0.2–6.8 km that had sufficient volume for both TOC and speciated organic composition analysis. Species included monocarboxylic acids (glycolate, acetate, formate, and pyruvate), dicarboxylic acids (glutarate, adipate, succinate, maleate, and oxalate), methanesulfonate (MSA), and dimethylamine (DMA). TOC values range between 0.018–13.660 ppm C with a mean of 0.902 ppm C. The highest TOC values are observed below 2 km with a general reduction aloft. An exception is samples impacted by biomass burning for which TOC remains enhanced as high as 6.5 km (7.048 ppm C). Estimated total organic matter derived from TOC contributes a mean of 30.7 % to total measured mass (inorganics + organics). Speciated organics contribute (on carbon mass basis) an average of 30.0 % to TOC in the study region, and account for an average of 10.3 % to total measured mass. The order of the average contribution of species to TOC, in decreasing contribution of carbon mass, is as follows: acetate (14.7 ± 20.5 %), formate (5.4 ± 9.3 %), oxalate (2.8 ± 4.3 %), DMA (1.7 ± 6.3 %), succinate (1.6 ± 2.4 %), pyruvate (1.3 ± 4.5 %), glycolate (1.3 ± 3.7 %), adipate (1.0 ± 3.6 %), MSA (0.1 ± 0.1 %), glutarate (0.1 ± 0.2 %), maleate (< 0.1 ± 0.1 %). Approximately 70 % of TOC remains unaccounted for, thus highlighting the complex nature of organics in the study region; samples collected in biomass burning plumes have up to 95.6 % of unaccounted TOC mass based on the species detected. Consistent with other regions, monocarboxylic acids dominate the speciated organic mass (~75 %) and are about four times in greater abundance than dicarboxylic acids. Samples are categorized into four cases based on back-trajectory history revealing source-independent similarity between the bulk contributions of monocarboxylic and dicarboxylic acids to TOC (16.03 %–23.66 % and 3.70 %–8.75 %, respectively). Furthermore, acetate, formate, succinate, glutarate, pyruvate, oxalate, and MSA are especially enhanced during biomass burning periods, attributed to peat emissions transported from Sumatra and Borneo. Lastly, dust (Ca2+) and sea salt (Na+/Cl−) tracers exhibit strong correlations with speciated organics, thus supporting how coarse aerosol surfaces interact with these water-soluble organics.

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Speciation of “brown” carbon in cloud water impacted by agricultural biomass burning in eastern China

Journal of Geophysical Research Atmospheres ◽

10.1002/jgrd.50561 ◽

2013 ◽

Vol 118 (13) ◽

pp. 7389-7399 ◽

Cited By ~ 125

Author(s):

Yury Desyaterik ◽

Yele Sun ◽

Xinhua Shen ◽

Taehyoung Lee ◽

Xinfeng Wang ◽

...

Keyword(s):

Biomass Burning ◽

Eastern China ◽

Cloud Water ◽

Brown Carbon ◽

Agricultural Biomass

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Total organic carbon and the contribution from speciated organics in cloud water: airborne data analysis from the CAMP<sup>2</sup>Ex field campaign

Atmospheric Chemistry and Physics ◽

10.5194/acp-21-14109-2021 ◽

2021 ◽

Vol 21 (18) ◽

pp. 14109-14129

Author(s):

Connor Stahl ◽

Ewan Crosbie ◽

Paola Angela Bañaga ◽

Grace Betito ◽

Rachel A. Braun ◽

...

Keyword(s):

Organic Carbon ◽

Total Organic Carbon ◽

Biomass Burning ◽

Dicarboxylic Acids ◽

Cloud Water ◽

Water Soluble ◽

Monocarboxylic Acids ◽

Study Region ◽

Carbon Mass ◽

Measured Mass

Abstract. This work focuses on total organic carbon (TOC) and contributing species in cloud water over Southeast Asia using a rare airborne dataset collected during NASA's Cloud, Aerosol and Monsoon Processes Philippines Experiment (CAMP2Ex), in which a wide variety of maritime clouds were studied, including cumulus congestus, altocumulus, altostratus, and cumulus. Knowledge of TOC masses and their contributing species is needed for improved modeling of cloud processing of organics and to understand how aerosols and gases impact and are impacted by clouds. This work relies on 159 samples collected with an axial cyclone cloud-water collector at altitudes of 0.2–6.8 km that had sufficient volume for both TOC and speciated organic composition analysis. Species included monocarboxylic acids (glycolate, acetate, formate, and pyruvate), dicarboxylic acids (glutarate, adipate, succinate, maleate, and oxalate), methanesulfonic acid (MSA), and dimethylamine (DMA). TOC values range between 0.018 and 13.66 ppm C with a mean of 0.902 ppm C. The highest TOC values are observed below 2 km with a general reduction aloft. An exception is samples impacted by biomass burning for which TOC remains enhanced at altitudes as high as 6.5 km (7.048 ppm C). Estimated total organic matter derived from TOC contributes a mean of 30.7 % to total measured mass (inorganics + organics). Speciated organics contribute (on a carbon mass basis) an average of 30.0 % to TOC in the study region and account for an average of 10.3 % to total measured mass. The order of the average contribution of species to TOC, in decreasing contribution of carbon mass, is as follows (±1 standard deviation): acetate (14.7 ± 20.5 %), formate (5.4 ± 9.3 %), oxalate (2.8 ± 4.3 %), DMA (1.7 ± 6.3 %), succinate (1.6 ± 2.4 %), pyruvate (1.3 ± 4.5 %), glycolate (1.3 ± 3.7 %), adipate (1.0 ± 3.6 %), MSA (0.1 ± 0.1 %), glutarate (0.1 ± 0.2 %), and maleate (< 0.1 ± 0.1 %). Approximately 70 % of TOC remains unaccounted for, highlighting the complex nature of organics in the study region; in samples collected in biomass burning plumes, up to 95.6 % of TOC mass is unaccounted for based on the species detected. Consistent with other regions, monocarboxylic acids dominate the speciated organic mass (∼ 75 %) and are about 4 times more abundant than dicarboxylic acids. Samples are categorized into four cases based on back-trajectory history, revealing source-independent similarity between the bulk contributions of monocarboxylic and dicarboxylic acids to TOC (16.03 %–23.66 % and 3.70 %–8.75 %, respectively). Furthermore, acetate, formate, succinate, glutarate, pyruvate, oxalate, and MSA are especially enhanced during biomass burning periods, which is attributed to peat emissions transported from Sumatra and Borneo. Lastly, dust (Ca2+) and sea salt (Na+/Cl-) tracers exhibit strong correlations with speciated organics, supporting how coarse aerosol surfaces interact with these water-soluble organics.

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Estimating the open biomass burning emissions in Central and Eastern China from 2003 to 2015 based on satellite observation

10.5194/acp-2018-282 ◽

2018 ◽

Author(s):

Jian Wu ◽

Shaofei Kong ◽

Fangqi Wu ◽

Yi Cheng ◽

Shurui Zheng ◽

...

Keyword(s):

Biomass Burning ◽

Annual Variation ◽

Eastern China ◽

Satellite Observation ◽

Pollutant Emissions ◽

Pollutant Emission ◽

Burned Area ◽

Management Policies ◽

Straw Burning ◽

Grassland Fire

Abstract. Open biomass burning (OBB) has significant impacts on air pollution, climate change and potential human health. OBB has raised wide attention but with few focus on the annual variation of pollutant emission. Central and Eastern China (CEC) is one of the most polluted regions in China. This study aims to provide a state-of the-art estimation of the pollutant emissions from OBB in CEC from 2003 to 2015, by adopting the satellite observation dataset (the burned area product (MCD64Al) and the active fire product (MCD14 ML)), local biomass data (updated biomass loading data and high-resolution vegetation data) and local emission factors. Monthly emissions of pollutants were estimated and allocated into a 1 × 1 km spatial grid for four types of OBB including grassland, shrubland, forest and cropland. From 2003 to 2015, the emissions from forest, shrubland and grassland fire burning had a minor annual variation whereas the emissions from crop straw burning steadily increased. The cumulative emissions of OC, EC, CH4, NOX, NMVOC, SO2, NH3, CO, CO2 and PM2.5 were 3.64 × 103, 2.87 × 102, 3.05 × 103, 1.82 × 103, 6.4 × 103, 2.12 × 102, 4.67 × 103, 4.59 × 104, 9.39 × 105 and 4.13 × 102 Gg in these years, respectively. For cropland, corn straw burning was the largest contributor for all pollutant emissions, by 84 %–96 %. Among the forest, shrubland, grassland fire burning, forest fire burning emissions contributed the most and emissions from grassland fire was negligible due to few grass coverage in this region. High pollutant emissions were populated in the connection area of Shandong, Henan, Jiangsu and Anhui, with emission intensity higher than 100 ton per pixel, which was related to the frequent agricultural activities in these regions. The monthly emission peak of pollutants occurred in summer and autumn harvest periods including May, June, September and October, at which period ~ 50 % of pollutants were emitted for OBB. This study highlights the importance in controlling the crops straw burning emission. From December to March of the next year, the crop residue burning emissions decreased, while the emissions from forest, shrubland and grassland exhibited their highest values, leading to another small peak emissions of pollutants. Obvious regional differences in seasonal variations of OBB were observed due to different local biomass types and environmental conditions. Rural population, agricultural output, local burning habits, anthropological activities and management policies are all influence factors for OBB emissions. The successful adoption of double satellite dataset for long term estimation of pollutants from OBB with a high spatial resolution can support the assessing of OBB on regional air-quality, especially for harvest periods or dry seasons. It is also useful to evaluate the effects of annual OBB management policies in different regions.

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Colorado air quality impacted by long-range-transported aerosol: a set of case studies during the 2015 Pacific Northwest fires

Atmospheric Chemistry and Physics ◽

10.5194/acp-16-12329-2016 ◽

2016 ◽

Vol 16 (18) ◽

pp. 12329-12345 ◽

Cited By ~ 6

Author(s):

Jessie M. Creamean ◽

Paul J. Neiman ◽

Timothy Coleman ◽

Christoph J. Senff ◽

Guillaume Kirgis ◽

...

Keyword(s):

Air Quality ◽

Case Studies ◽

Pacific Northwest ◽

Long Range ◽

Biomass Burning ◽

Forest Fires ◽

Surface Radiation ◽

Cloud Formation ◽

Synoptic Scale ◽

Transport Pathways

Abstract. Biomass burning plumes containing aerosols from forest fires can be transported long distances, which can ultimately impact climate and air quality in regions far from the source. Interestingly, these fires can inject aerosols other than smoke into the atmosphere, which very few studies have evidenced. Here, we demonstrate a set of case studies of long-range transport of mineral dust aerosols in addition to smoke from numerous fires (including predominantly forest fires and a few grass/shrub fires) in the Pacific Northwest to Colorado, US. These aerosols were detected in Boulder, Colorado, along the Front Range using beta-ray attenuation and energy-dispersive X-ray fluorescence spectroscopy, and corroborated with satellite-borne lidar observations of smoke and dust. Further, we examined the transport pathways of these aerosols using air mass trajectory analysis and regional- and synoptic-scale meteorological dynamics. Three separate events with poor air quality and increased mass concentrations of metals from biomass burning (S and K) and minerals (Al, Si, Ca, Fe, and Ti) occurred due to the introduction of smoke and dust from regional- and synoptic-scale winds. Cleaner time periods with good air quality and lesser concentrations of biomass burning and mineral metals between the haze events were due to the advection of smoke and dust away from the region. Dust and smoke present in biomass burning haze can have diverse impacts on visibility, health, cloud formation, and surface radiation. Thus, it is important to understand how aerosol populations can be influenced by long-range-transported aerosols, particularly those emitted from large source contributors such as wildfires.

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Nutrient status and winter hardiness of red spruce foliage

Canadian Journal of Forest Research ◽

10.1139/x89-115 ◽

1989 ◽

Vol 19 (6) ◽

pp. 754-758 ◽

Cited By ~ 24

Author(s):

Richard M. Klein ◽

Timothy D. Perkins ◽

Helen L. Myers

Keyword(s):

Inorganic Nitrogen ◽

Sufficient Conditions ◽

Nutrient Status ◽

Cloud Water ◽

Winter Hardiness ◽

Red Spruce ◽

Anthropogenic Sources ◽

Freezing Injury ◽

Ion Leakage ◽

Anthropogenic Nitrogen

Increased ecosystem loading with inorganic nitrogen compounds derived from anthropogenic sources has been proposed to prolong vegetative growth of spruce, rendering them more susceptible to winter injury. Severely nutrient-deficient 4-year-old red spruce (Picearubens Sarg.) seedlings and adequately fertilized seedlings were provided with synthetic cloud water lacking or containing nitrate, ammonium, or both, for a full growing season, and then exposed to normal winter chilling. Needles from these seedlings were stressed at −25 or −30 °C, and freezing injury was measured as ion leakage. Cloud water condensates had no effect on hardiness of needles of either nutrient status. Initially nutrient-sufficient seedlings transferred to nutrient-deficient conditions also exhibited no change in hardiness. Severely nutrient-deficient seedlings had needles that were significantly more sensitive to winter injury than seedlings under nutrient-sufficient conditions. Improving the nutrient status of initially nitrogen-deficient seedlings reduced their sensitivity to freezing injury. Based upon experimental results and consideration of the amounts of inorganic nitrogen reaching upper-elevation conifer forests, there is no evidence to support the hypothesis that anthropogenic nitrogen supplies significantly reduce winter hardiness of spruce foliage. It is improbable that winter injury due to elevated anthropogenic nitrogen is a causal factor in contemporary forest decline.

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Modelling the ecosystem effects of nitrogen deposition: Model of Ecosystem Retention and Loss of Inorganic Nitrogen (MERLIN

Hydrology and Earth System Sciences ◽

10.5194/hess-1-137-1997 ◽

1997 ◽

Vol 1 (1) ◽

pp. 137-158 ◽

Cited By ~ 22

Author(s):

B. J. Cosby ◽

R. C. Ferrier ◽

A. Jenkins ◽

B. A. Emmett ◽

R. F. Wright ◽

...

Keyword(s):

Nitrogen Deposition ◽

Soil Solution ◽

Nitrogen Uptake ◽

Inorganic Nitrogen ◽

Balance Model ◽

Litter Production ◽

Catchment Scale ◽

Exchange Constants ◽

External Sources ◽

Carbon Productivity

Abstract. A catchment-scale mass-balance model of linked carbon and nitrogen cycling in ecosystems has been developed for simulating leaching losses of inorganic nitrogen. The model (MERLIN) considers linked biotic and abiotic processes affecting the cycling and storage of nitrogen. The model is aggregated in space and time and contains compartments intended to be observable and/or interpretable at the plot or catchment scale. The structure of the model includes the inorganic soil, a plant compartment and two soil organic compartments. Fluxes in and out of the ecosystem and between compartments are regulated by atmospheric deposition, hydrological discharge, plant uptake, litter production, wood production, microbial immobilization, mineralization, nitrification, and denitrification. Nitrogen fluxes are controlled by carbon productivity, the C:N ratios of organic compartments and inorganic nitrogen in soil solution. Inputs required are: 1) temporal sequences of carbon fluxes and pools- 2) time series of hydrological discharge through the soils, 3) historical and current external sources of inorganic nitrogen; 4) current amounts of nitrogen in the plant and soil organic compartments; 5) constants specifying the nitrogen uptake and immobilization characteristics of the plant and soil organic compartments; and 6) soil characteristics such as depth, porosity, bulk density, and anion/cation exchange constants. Outputs include: 1) concentrations and fluxes of NO3 and NH4 in soil solution and runoff; 2) total nitrogen contents of the organic and inorganic compartments; 3) C:N ratios of the aggregated plant and soil organic compartments; and 4) rates of nitrogen uptake and immobilization and nitrogen mineralization. The behaviour of the model is assessed for a combination of land-use change and nitrogen deposition scenarios in a series of speculative simulations. The results of the simulations are in broad agreement with observed and hypothesized behaviour of nitrogen dynamics in growing forests receiving nitrogen deposition.

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Transport, mixing and feedback of dust, biomass burning and anthropogenic pollutants in eastern Asia: a case study

Atmospheric Chemistry and Physics ◽

10.5194/acp-18-16345-2018 ◽

2018 ◽

Vol 18 (22) ◽

pp. 16345-16361 ◽

Cited By ~ 9

Author(s):

Derong Zhou ◽

Ke Ding ◽

Xin Huang ◽

Lixia Liu ◽

Qiang Liu ◽

...

Keyword(s):

Air Pollution ◽

Biomass Burning ◽

Southern China ◽

Eastern China ◽

Measurement Data ◽

Lower Troposphere ◽

Climate Impacts ◽

Eastern Asia ◽

Pollution Episode ◽

The Yrd

Abstract. Anthropogenic fossil fuel (FF) combustion, biomass burning (BB) and desert dust are the main sources of air pollutants around the globe but are particularly intensive and important for air quality in Asia in spring. In this study, we investigate the vertical distribution, transport characteristics, source contribution and meteorological feedback of these aerosols in a unique pollution episode that occurred in eastern Asia based on various measurement data and modeling methods. In this episode, the Yangtze River Delta (YRD) in eastern China experienced persistent air pollution, dramatically changing from secondary fine particulate pollution to dust pollution in late March 2015. The Eulerian and Lagrangian models were conducted to investigate the vertical structure, transport characteristics and mechanisms of the multi-scale, multisource and multiday air pollution episode. The regional polluted continental aerosols mainly accumulated near the surface, mixed with dust aerosol downwash from the upper planetary boundary layer (PBL) and middle–lower troposphere (MLT), and further transported by large-scale cold fronts and warm conveyor belts. BB smoke from Southeast Asia was transported by westerlies around the altitude of 3 km from southern China, was further mixed with dust and FF aerosols in eastern China and experienced long-range transport over the Pacific. These pollutants could all be transported to the YRD region and cause a structure of multilayer pollution there. These pollutants could also cause significant feedback with MLT meteorology and then enhance local anthropogenic pollution. This study highlights the importance of intensive vertical measurement in eastern China and the downwind Pacific Ocean and raises the need for quantitative understanding of environmental and climate impacts of these pollution sources.

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