Vertical distribution of water-soluble, sea salt, and dust aerosols in the planetary boundary layer estimated from two-wavelength backscatter and one-wavelength polarization lidar measurements in Guangzhou and Beijing, China

2010 ◽  
Vol 96 (4) ◽  
pp. 602-611 ◽  
Author(s):  
Tomoaki Nishizawa ◽  
Nobuo Sugimoto ◽  
Ichiro Matsui ◽  
Atsushi Shimizu ◽  
Xingang Liu ◽  
...  
2020 ◽  
Author(s):  
Wanyu Zhao ◽  
Hong Ren ◽  
Kimitaka Kawamura ◽  
Huiyun Du ◽  
Xueshun Chen ◽  
...  

Abstract. Vertical distribution of dicarboxylic acids, oxoacids, α-dicarbonyls, and other organic tracer compounds in fine aerosols (PM2.5) was investigated from the ground surface (8 m) to 260 m at a 325-meter meteorological tower in Beijing in the summer of 2015. Results showed that the concentrations of oxalic acid (C2), the predominant diacid, were more abundant at 120 m (210 ± 154 ng m−3) and 260 m (220 ± 140 ng m−3) than those at the ground level (160 ± 90 ng m−3). Concentrations of phthalic acid (Ph) decreased with the increase of heights, demonstrating that the vehicular exhausts at the ground surface was the main contributor. Positive correlations were noteworthy for C2/total diacids with mass ratios of C2 to main oxoacids (Pyr, ωC2) and α-dicarbonyls (Gly, MeGly) in polluted days (0.42 ≤ r2 ≤ 0.65), especially at the ground level. In clean days, the ratios of carbon content in oxalic acid to water soluble organic carbon (C2-C/WSOC) showed larger values at 120 m and 260 m than those at the ground surface. However, in polluted days, the C2-C/WSOC ratio mainly reached its maximum at the ground level. These phenomena may indicate the enhanced contribution of aqueous-phase oxidation to oxalic acid in polluted days. Combined with the influence of wind field, total diacids, oxoacids and α-dicarbonyls decreased by 22 %–58 % under the control on anthropogenic activities during the 2015 Victory Parade period. Furthermore, the PMF results showed that the secondary formation routes (secondary sulfate formation and secondary nitrate formation) were the dominant contributors (37–44 %) to organic acids, followed by biomass burning (25–30 %) and motor vehicles (18–24 %). In this study, the organic acids at the ground level were largely associated with local traffic emissions, while the long-range atmospheric transport followed by photochemical aging contributed more to diacids and related compounds in the boundary layer over Beijing than the ground surface.


2013 ◽  
Vol 13 (10) ◽  
pp. 27971-28016 ◽  
Author(s):  
H. Geng ◽  
H. J. Hwang ◽  
X. Liu ◽  
S. Dong ◽  
C.-U. Ro

Abstract. This is the first study of Asian dust storm (ADS) particles collected in Beijing, China and Incheon, Korea during the same spring ADS event. Using a seven-stage May impactor and a quantitative electron probe X-ray microanalysis (ED-EPMA, also known as low-Z particle EPMA), we examined the composition and morphology of 4200 aerosol particles at stages 1–6 (with a size cut-off of 16, 8, 4, 2, 1, and 0.5 μm in equivalent aerodynamic diameter, respectively) collected during an ADS event on 28–29 April 2005. The results showed that there were large differences in the chemical compositions between particles in sample S1 collected in Beijing immediately after the peak time of the ADS and in samples S2 and S3, which were collected in Incheon approximately 5 h and 24 h later, respectively. In sample S1, mineral dust particles accounted for more than 88% in relative number abundance at stages 1–5, and organic carbon (OC) and reacted NaCl-containing particles accounted for 24% and 32%, respectively, at stage 6. On the other hand, in samples S2 and S3, in addition to approximately 60% mineral dust, many sea salt particles reacted with airborne SO2 and NOx, often mixed with mineral dust, were encountered at stages 1–5, and (C, N, O, S)-rich particles (likely a mixture of water-soluble organic carbon with (NH4)2SO4 and NH4NO3) and K-containing particles were abundantly observed at stage 6. This suggests that the secondary aerosols and the internal mixture of mineral dust with sea spray aerosol increased when the ADS particles passed over the Yellow Sea. In the reacted or aged mineral dust and sea salt particles, nitrate-containing and both nitrate- and sulfate-containing species vastly outnumbered the sulfate-containing species, implying that ambient nitrogen oxides had a greater influence on the atmospheric particles during the ADS episode than SO2. In addition to partially- or totally-reacted CaCO3, reacted or aged Mg-containing aluminosilicates (likely including amesite, allophite, vermiculite, illite, and montmorillonite) were observed frequently in samples S2 and S3; and furthermore, both the atomic concentration ratios of [Mg]/[Al] and [Mg]/[Si] were elevated compared to that in sample S1. This shows that a great evolution or aging process must have occurred on the mineral dust. This indicates that the number abundance, reactivity with gaseous pollutants, and ratios of [Mg]/[Al] and [Mg]/[Si] of Mg-containing aluminosilicates are promising indices of the aging process of ADS particles during long-range transport.


Tellus B ◽  
2011 ◽  
Vol 63 (4) ◽  
Author(s):  
Silke Groß ◽  
Josef Gasteiger ◽  
Volker Freudenthaler ◽  
Matthias Wiegner ◽  
Alexander Geiß ◽  
...  

2020 ◽  
Vol 20 (11) ◽  
pp. 6435-6453 ◽  
Author(s):  
Shengzhen Zhou ◽  
Luolin Wu ◽  
Junchen Guo ◽  
Weihua Chen ◽  
Xuemei Wang ◽  
...  

Abstract. Many studies have recently been done on understanding the sources and formation mechanisms of atmospheric aerosols at ground level. However, vertical profiles and sources of size-resolved particulate matter within the urban boundary layer are still lacking. In this study, vertical distribution characteristics of size-segregated particles were investigated at three observation platforms (ground level, 118 m, and 488 m) on the 610 m high Canton Tower in Guangzhou, China. Size-segregated aerosol samples were simultaneously collected at the three levels in autumn and winter. Major aerosol components, including water-soluble ions, organic carbon, and elemental carbon, were measured. The results showed that daily average fine-particle concentrations generally decreased with height. Concentrations of sulfate and ammonium in fine particles displayed shallow vertical gradients, and nitrate concentrations increased with height in autumn, while the chemical components showed greater variations in winter than in autumn. The size distributions of sulfate and ammonium in both seasons were characterized by a dominant unimodal mode with peaks in the size range of 0.44–1.0 µm. In autumn, the nitrate size distribution was bimodal, peaking at 0.44–1.0 and 2.5–10 µm, while in winter it was unimodal, implying that the formation mechanisms for nitrate particles were different in the two seasons. Our results suggest that the majority of the sulfate and nitrate is formed from aqueous-phase reactions, and we attribute coarse-mode nitrate formation at the measurement site to the heterogeneous reactions of gaseous nitric acid on existing sea-derived coarse particles in autumn. Case studies further showed that atmospheric aqueous-phase and heterogeneous reactions could be important mechanisms for sulfate and nitrate formation, which, in combination with adverse weather conditions such as temperature inversion and calm wind, led to haze formation during autumn and winter in the Pearl River Delta (PRD) region.


2016 ◽  
Vol 16 (17) ◽  
pp. 10831-10845 ◽  
Author(s):  
Marie Boichu ◽  
Isabelle Chiapello ◽  
Colette Brogniez ◽  
Jean-Christophe Péré ◽  
Francois Thieuleux ◽  
...  

Abstract. The 2014–2015 Holuhraun lava-flood eruption of Bárðarbunga volcano (Iceland) emitted prodigious amounts of sulfur dioxide into the atmosphere. This eruption caused a large-scale episode of air pollution throughout Western Europe in September 2014, the first event of this magnitude recorded in the modern era. We gathered chemistry-transport simulations and a wealth of complementary observations from satellite sensors (OMI, IASI), ground-based remote sensing (lidar, sunphotometry, differential optical absorption spectroscopy) and ground-level air quality monitoring networks to characterize both the spatial-temporal distributions of volcanic SO2 and sulfate aerosols as well as the dynamics of the planetary boundary layer. Time variations of dynamical and microphysical properties of sulfate aerosols in the aged low-tropospheric volcanic cloud, including loading, vertical distribution, size distribution and single scattering albedo, are provided. Retrospective chemistry-transport simulations at low horizontal resolution (25 km  ×  25 km) capture the correct temporal dynamics of this far-range air pollution event but fail to reproduce the correct magnitude of SO2 concentration at ground-level. Simulations at higher spatial resolution, relying on two nested domains with finest resolution of 7.3 km  ×  7.3 km, improve substantially the far-range vertical distribution of the volcanic cloud and subsequently the description of ground-level SO2 concentrations. However, remaining discrepancies between model and observations are shown to result from an inaccurate representation of the planetary boundary layer (PBL) dynamics. Comparison with lidar observations points out a systematic under-estimation of the PBL height by the model, whichever the PBL parameterization scheme. Such a shortcoming impedes the capture of the overlying Bárðarbunga cloud into the PBL at the right time and in sufficient quantities. This study therefore demonstrates the key role played by the PBL dynamics in accurately modelling large-scale volcanogenic air pollution.


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