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Formation and evolution mechanism of regional haze: a case study in the megacity Beijing, China

The main objective of this study is to investigate the formation and evolution mechanism of the regional haze in megacity Beijing by analyzing the process of a severe haze that occurred 20–27 September 2011. Mass concentration and size distribution of aerosol particles as well as aerosol optical properties were concurrently measured at the Beijing urban atmospheric environment monitoring station. Gaseous pollutants (SO2, NO-NO2-NOx, O3, CO) and meteorological parameters (wind speed, wind direction, and relative humidity) were simultaneously monitored. Meanwhile, aerosol spatial distribution and the height of planetary boundary layer (PBL) were retrieved from the signal of satellite and LIDAR (light detection and ranging). Concentrations of NO, NO2, SO2, O3, and CO observed during 23–27 September had exceeded the national ambient air quality standards for residents. The mass concentration of PM2.5 gradually accumulated during the measurement and reached at 220 μg m−3 on 26 September, and the corresponding atmospheric visibility was only 1.1 km. The daily averaged AOD in Beijing increased from ~ 0.16 at λ = 500 nm on 22 September and reached ~ 3.5 on 26 September. The key factors that affected the formation and evolution of this haze episode were stable anti-cyclone synoptic conditions at the surface, decreasing of the height of PBL, heavy pollution emissions from urban area, number and size evolution of aerosols, and hygroscopic growth for aerosol scattering. This case study may provide valuable information for the public to recognize the formation mechanism of the regional haze event over the megacity, which is also useful for the government to adopt scientific approach to forecast and eliminate the occurrence of regional haze in China.
Evaluation of a new middle-lower tropospheric CO2 product using data assimilation

Atmospheric CO2 retrievals with peak sensitivity in the mid- to lower troposphere from the Atmospheric Infrared Sounder (AIRS) have been assimilated into the GEOS-5 (Goddard Earth Observing System Model, Version 5) constituent assimilation system for the period 1 January 2005 to 31 December 2006. A corresponding model simulation, using identical initial conditions, circulation, and CO2 boundary fluxes was also completed. The analyzed and simulated CO2 fields are compared with surface measurements globally and aircraft measurements over North America. Surface level monthly mean CO2 values show a marked improvement due to the assimilation in the Southern Hemisphere, while less consistent improvements are seen in the Northern Hemisphere. Mean differences with aircraft observations are reduced at all levels, with the largest decrease occurring in the mid-troposphere. The difference standard deviations are reduced slightly at all levels over the ocean, and all levels except the surface layer over land. These initial experiments indicate that the used channels contain useful information on CO2 in the middle to lower troposphere. However, the benefits of assimilating these data are reduced over the land surface, where concentrations are dominated by uncertain local fluxes and where the observation density is quite low. Away from these regions, the study demonstrates the power of the data assimilation technique for evaluating data that are not co-located, in that the improvements in mid-tropospheric CO2 by the sparsely distributed partial-column retrievals are transported by the model to the fixed in situ surface observation locations in more remote areas.
ACE-FTS observations of pyrogenic trace species in boreal biomass burning plumes during BORTAS

To further our understanding of the effects of biomass burning emissions on atmospheric composition, the BORTAS campaign (BOReal forest fires on Tropospheric oxidants over the Atlantic using Aircraft and Satellites) was conducted on 12 July to 3 August 2011 during the boreal forest fire season in Canada. The simultaneous aerial, ground and satellite measurement campaign sought to record instances of boreal biomass burning to measure the tropospheric volume mixing ratios (VMRs) of short- and long-lived trace molecular species from biomass burning emissions. The goal was to investigate the connection between the composition and the distribution of these pyrogenic outflows and their resulting perturbation to atmospheric chemistry, with particular focus on oxidant species to determine the overall impact on the oxidizing capacity of the free troposphere. Measurements of pyrogenic trace species in boreal biomass burning plumes were made by the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) onboard the Canadian Space Agency (CSA) SCISAT-1 satellite during the BORTAS campaign. Even though biomass burning emissions are typically confined to the boundary layer, outflows are often injected into the upper troposphere by isolated convection and fire-related convective processes, thus allowing space-borne instruments to measure these pyrogenic outflows. An extensive set of 14 molecules – CH3OH, C2H2, C2H6, C3H6O, CO, HCN, HCOOH, HNO3, H2CO, NO, NO2, OCS, O3, and PAN – have been analysed. Included in this analysis is the calculation of age-dependent sets of enhancement ratios for each of the species originating from fires in North America (Canada, Alaska) and Siberia for a period of up to 7 days. Ratio values for the shorter lived primary pyrogenic species decrease over time primarily due to oxidation by the OH radical as the plume ages and values for longer lived species such as HCN and C2H6 remain relatively unchanged. Increasing negative values are observed for the oxidant species, including O3, indicating a destruction process in the plume as it ages such that concentrations of the oxidant species have dropped below their off-plume values. Results from previous campaigns have indicated that values for the molar ratios of ΔO3 /ΔO obtained from the measurements of the pyrogenic outflow from boreal fires are highly variable and range from negative to positive, irrespective of plume age. This variability has been attributed to pollution effects where the pyrogenic outflows have mixed with either local urban NOx emissions or pyrogenic emissions from the long-range transport of older plumes, thus affecting the production of O3 within the plumes. The results from this study have identified another potential cause of the variability in O3 concentrations observed in the measurements of biomass burning emissions, where evidence of stratosphere–troposphere exchange due to the pyroconvective updrafts from fires has been identified. Perturbations caused by the lofted emissions in these fire-aided convective processes may result in the intrusion of stratospheric air masses into the free troposphere and subsequent mixing of stratospheric O3 into the pyrogenic outflows causing fluctuations in observed ΔO3/ΔCO molar ratios.
Improved SAGE II cloud/aerosol categorization and observations of the Asian tropopause aerosol layer: 1989–2005

We describe the challenges associated with the interpretation of extinction coefficient measurements by the Stratospheric Aerosol and Gas Experiment (SAGE II) in the presence of clouds. In particular, we have found that tropospheric aerosol analyses are highly dependent on a robust method for identifying when clouds affect the measured extinction coefficient. Herein, we describe an improved cloud identification method that appears to capture cloud/aerosol events more effectively than early methods. In addition, we summarize additional challenges to observing the Asian Tropopause Aerosol Layer (ATAL) using SAGE II observations. Using this new approach, we perform analyses of the upper troposphere, focusing on periods in which the UTLS (upper troposphere/lower stratosphere) is relatively free of volcanic material (1989–1990 and after 1996). Of particular interest is the Asian monsoon anticyclone where CALIPSO (Cloud-Aerosol Lidar Pathfinder Satellite Observations) has observed an aerosol enhancement. This enhancement, called the ATAL, has a similar morphology to observed enhancements in long-lived trace gas species like CO. Since the CALIPSO record begins in 2006, the question of how long this aerosol feature has been present requires a new look at the long-lived SAGE II data sets despite significant hurdles to its use in the subtropical upper troposphere. We find that there is no evidence of ATAL in the SAGE II data prior to 1998. After 1998, it is clear that aerosol in the upper troposphere in the ATAL region is substantially enhanced relative to the period before that time. In addition, the data generally supports the presence of the ATAL beginning in 1999 and continuing through the end of the mission, though some years (e.g., 2003) are complicated by the presence of episodic enhancements most likely of volcanic origin.
Laser filament-induced aerosol formation

Using the aerosol and cloud simulation chamber AIDA, we investigated the laser filament induced particle formation in ambient air, humid synthetic air, humid nitrogen, argon–oxygen mixture, and pure argon in order to simulate the particle formation under realistic atmospheric conditions as well as to investigate the influence of typical gas-phase atmospheric constituents on the particle formation. Terawatt laser plasma filaments generated new particles in the size range 3 to 130 nm with particle production rates ranging from 1 × 107 to 5 × 109 cm−3 plasma s−1 for the given experimental conditions. In all cases the particle formation rates increased exponentially with the water content of the gas mixture. Furthermore, the presence of a few ppb of trace gases like SO2 and α-pinene clearly enhanced the particle yield by number, the latter also by mass. Our findings suggest that new particle formation is efficiently supported by oxidized species like acids generated by the photoionization of both major and minor components of the air, including N2, NH3, SO2 and organics.
Characteristics of concentrations and chemical compositions for PM2.5 in the region of Beijing, Tianjin, and Hebei, China

In order to study the temporal and spatial variations of PM2.5 and its chemical compositions in the region of Beijing, Tianjin, and Hebei (BTH), PM2.5 samples were collected at four urban sites in Beijing (BJ), Tianjin (TJ), Shijiazhuang (SJZ), and Chengde (CD), and also one site at Shangdianzi (SDZ) regional background station over four seasons from 2009 to 2010. The samples were weighted for mass concentrations and analyzed in the laboratory for chemical profiles of 19 elements (Al, As, Ba, Ca, Cd, Co, Cr, Cu, Fe, K, Mg, Mn, Ni, P, Pb, Sr, Ti, V, and Zn), eight water-soluble inorganic ions (Na+, NH4+, K+, Mg2+, Ca2+, Cl−, NO3−, and SO42−, and carbon fractions (OC and EC). The concentrations of PM2.5 and its major chemical species were season dependent and showed spatially similar characteristics in the plain area of BTH. The average annual concentrations of PM2.5 were 71.8–191.2 μg m−3 at the five sites, with more than 90% of sampling days exceeding 50 μg m−3 at BJ, TJ, and SJZ. PM2.5 pollution was most serious at SJZ, and the annual concentrations of PM2.5, secondary inorganic ions, OC, EC, and most crustal elements were all highest. Due to stronger photochemical oxidation, the sum of concentrations of secondary inorganic ions (NH4+, NO3−, and SO42− was highest in the summer at SDZ, BJ, TJ, and CD. Analysis of electric charges of water-soluble inorganic ions indicated the existence of nitric acid or hydrochloric acid in PM2.5. For all five sites, the concentrations of OC, EC and also secondary organic carbon (SOC) in the spring and summer were lower than those in the autumn and winter. SOC had more percentages of increase than primary organic carbon (POC) during the winter. The sums of crustal elements (Al, Ca, Fe, Mg, Ti, Ba, and Sr) were higher in the spring and autumn owing to more days with blowing or floating dust. The concentrations of heavy metals were at higher levels in the BTH area by comparison with other studies. In Shijiazhuang and Chengde, the PM2.5 pollution was dominated by coal combustion. Motor vehicle exhausts and coal combustion emissions both played important roles in Tianjin PM2.5 pollution. However, motor vehicle exhausts had played a more important role in Beijing owing to the reduction of coal consumption and sharp increase of cars in recent years. At SDZ, regional transportation of air pollutants from southern urban areas was significant.
On the export of reactive nitrogen from Asia: NOx partitioning and effects on ozone

The partitioning of reactive nitrogen (NOy was measured over the remote North Pacific during spring 2006. Aircraft observations of NO, NO2, total peroxy nitrates (ΣPNs), total alkyl and multi-functional nitrates (ΣANs) and nitric acid (HNO3, made between 25° and 55° N, confirm a controlling role for peroxyacyl nitrates in NOx production in aged Asian outflow. ΣPNs account for more than 60% of NOy above 5 km, while thermal dissociation limits their contribution to less than 10% in the lower troposphere. Using simultaneous observations of NOx, ΣPNs, ΣANs, HNO3 and average wind speed, we calculate the flux of reactive nitrogen through the meridional plane of 150° W (between 20° and 55° N) to be 0.007 ± 0.002 Tg N day−1, which provides an upper limit of 23 ± 6.5% on the transport efficiency of NOy from East Asia. Observations of NOx, and HOx are used to constrain a 0-D photochemical box model for the calculation of net photochemical ozone production or tendency (Δ O3) as a function of aircraft altitude and NOx concentrations. The model analysis indicates that the photochemical environment of the lower troposphere (altitude < 6 km) over the north Pacific is one of net O3 destruction, with an experimentally determined crossover point between net O3 destruction and net O3 production of 60 pptv NOx. Qualitative indicators of integrated net O3 production derived from simultaneous measurements of O3 and light alkanes (Parrish et al., 1992), also indicate that the north Pacific is, on average, a region of net O3 destruction.
Heterogeneous ice nucleation on phase-separated organic-sulfate particles: effect of liquid vs. glassy coatings

Atmospheric ice nucleation on aerosol particles relevant to cirrus clouds remains one of the least understood processes in the atmosphere. Upper tropospheric aerosols as well as sub-visible cirrus residues are known to be enhanced in both sulfates and organics. The hygroscopic phase transitions of organic-sulfate particles can have an impact on both the cirrus cloud formation mechanism and resulting cloud microphysical properties. In addition to deliquescence and efflorescence, organic-sulfate particles are known to undergo another phase transition known as liquid–liquid phase separation. The ice nucleation properties of particles that have undergone liquid–liquid phase separation are unknown. Here, Raman microscopy coupled with an environmental cell was used to study the low temperature deliquescence, efflorescence, and liquid–liquid phase separation behavior of 2 : 1 mixtures of organic polyols (1,2,6-hexanetriol and 1 : 1 1,2,6-hexanetriol + 2,2,6,6-tetrakis(hydroxymethyl)cyclohexanol) and ammonium sulfate from 240–265 K. Further, the ice nucleation efficiency of these organic-sulfate systems after liquid–liquid phase separation and efflorescence was investigated from 210–235 K. Raman mapping and volume-geometry analysis indicate that these particles contain solid ammonium sulfate cores fully engulfed in organic shells. For the ice nucleation experiments, we find that if the organic coatings are liquid, water vapor diffuses through the shell and ice nucleates on the ammonium sulfate core. In this case, the coatings minimally affect the ice nucleation efficiency of ammonium sulfate. In contrast, if the coatings become semi-solid or glassy, ice instead nucleates on the organic shell. Consistent with recent findings that glasses can be efficient ice nuclei, the phase-separated particles are nearly as efficient at ice nucleation as pure crystalline ammonium sulfate.
Organic and inorganic markers and stable C-, N-isotopic compositions of tropical coastal aerosols from megacity Mumbai: sources of organic aerosols and atmospheric processing

To better understand the sources of PM10 samples in Mumbai, India, aerosol chemical composition, i.e., total carbon (TC), organic carbon (OC), elemental carbon (EC), water-soluble organic carbon (WSOC), and inorganic ions were studied together with specific markers such as methanesulfonate (MSA), oxalic acid (C2), azelaic acid (C9), and levoglucosan. The results revealed that biofuel/biomass burning and fossil fuel combustion are the major sources of the Mumbai aerosols. Nitrogen-isotopic (δ15N) composition of aerosol total nitrogen, which ranged from 18.1 to 25.4&permil;, also suggests that biofuel/biomass burning is a predominate source in both the summer and winter seasons. Aerosol mass concentrations of major species increased 3–4 times in winter compared to summer, indicating enhanced emission from these sources in the winter season. Photochemical production tracers, C2 diacid and nssSO42−, do not show diurnal changes. Concentrations of C2 diacid and WSOC show a strong correlation (r2 = 0.95). In addition, WSOC to OC (or TC) ratios remain almost constant for daytime (0.37 &pm; 0.06 (0.28 &pm; 0.04)) and nighttime (0.38 &pm; 0.07 (0.28 &pm; 0.06)), suggesting that mixing of fresh secondary organic aerosols is not significant and the Mumbai aerosols are photochemically well processed. Concentrations of MSA and C9 diacid present a positive correlation (r2 = 0.75), indicating a marine influence on Mumbai aerosols in addition to local/regional influence. Backward air mass trajectory analyses further suggested that the Mumbai aerosols are largely influenced by long-range continental and regional transport. Stable C-isotopic ratios (δ13C) of TC ranged from −27.0 to −25.4&permil;, with slightly lower average (−26.5 &pm; 0.3&permil;) in summer than in winter (−25.9 &pm; 0.3&permil;). Positive correlation between WSOC/TC ratios and δ13C values suggested that the relative increment in 13C of wintertime TC may be caused by prolonged photochemical processing of organic aerosols in this season. This study suggests that in winter, the tropical aerosols are more aged due to longer residence time in the atmosphere than in summer aerosols. However, these conclusions are based on the analysis of a limited number of samples (n=25) and more information on this topic may be needed from other similar coastal sites in future.
Multi-season eddy covariance observations of energy, water and carbon fluxes over a suburban area in Swindon, UK

Eddy covariance measurements of the turbulent sensible heat, latent heat and carbon dioxide fluxes for 12 months (2011–2012) are reported for the first time for a suburban area in the UK. The results from Swindon are comparable to suburban studies of similar surface cover elsewhere but reveal large seasonal variability. Energy partitioning favours turbulent sensible heat during summer (midday Bowen ratio 1.4–1.6) and latent heat in winter (0.05–0.7). A significant proportion of energy is stored (and released) by the urban fabric and the estimated anthropogenic heat flux is small but non-negligible (0.5–0.9 MJ m−2 day−1). The sensible heat flux is negative at night and for much of winter daytimes, reflecting the suburban nature of the site (44% vegetation) and relatively low built fraction (16%). Latent heat fluxes appear to be water limited during a dry spring in both 2011 and 2012, when the response of the surface to moisture availability can be seen on a daily timescale. Energy and other factors are more relevant controls at other times; at night the wind speed is important. On average, surface conductance follows a smooth, asymmetrical diurnal course peaking at around 6–9 mm s−1, but values are larger and highly variable in wet conditions. The combination of natural (vegetative) and anthropogenic (emission) processes is most evident in the temporal variation of the carbon flux: significant photosynthetic uptake is seen during summer, whilst traffic and building emissions explain peak release in winter (9.5 g C m−2 day−1). The area is a net source of CO2 annually. Analysis by wind direction highlights the role of urban vegetation in promoting evapotranspiration and offsetting CO2 emissions, especially when contrasted against peak traffic emissions from sectors with more roads. Given the extent of suburban land use, these results have important implications for understanding urban energy, water and carbon dynamics.