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Pollution events observed during CARIBIC flights in the upper troposphere between South China and the Philippines

A strong pollution episode in the upper troposphere between South China and the Philippines was observed during CARIBIC flights in April 2007. Five pollution events were observed, where enhancements in aerosol and trace gas concentrations including CO, CO2, CH4, non-methane hydrocarbons (NMHCs) and halocarbons were observed along the flight tracks during four sequential flights. The importance of the contribution of biomass/biofuel burning was investigated using chemical tracers, emission factor analysis, back-trajectory analysis and satellite images. The Indochinese peninsula was identified as the probable source region of biomass/biofuel burning. However, enhancements in the urban/industrial tracer C2Cl4 during the events also indicate a substantial contribution from urban anthropogenic emissions. An estimation of the contribution of fossil fuel versus biomass/biofuel to the CO enhancement was made, indicating a biomass/biofuel burning contribution of ~54 to ~92% of the observed CO enhancements. Biomass/biofuel burning was found to be the most important source category during the sampling period.
Measurements of electric charge separated during the formation of rime by the accretion of supercooled droplets

In these experiments, the electric charge carried by single particles ejected from the surface of a graupel particle growing by riming was measured. Simulated graupel pellets were grown by accretion of supercooled water drops, at temperatures ranging from −2 to −10 °C in a wind tunnel at air velocities between 5 and 10 m s−1, with the goal of studying the charging of graupel pellets under conditions of secondary ice crystal production (Hallett-Mossop mechanism). The graupel, and induction rings upstream and downstream of the graupel, were connected to electrometers and analyzing circuits of sufficient sensitivity and speed to measure, correlate and display individual charging events. The results suggest that fewer than 1% of the ejected particles carry a measurable electric charge (>2 fC). Further, it was observed that the graupel pellets acquire a positive charge and the average charge of a single splinter ejected is −14 fC. This mechanism of ejection of charged particles seems adequate to account for a positive charge of around 1 pC that individual precipitation particles of mm-size could acquire in the lower part of the cloud, which in turn could contribute to the lower positive charge region of thunderstorms.
Recent increase in aerosol loading over the Australian arid zone

Collocated sun photometer and nephelometer measurements at Tinga Tingana in the Australian Outback over the decade 1997–2007 show a significant increase in aerosol loading following the onset of severe drought conditions in 2002. This increase is confined to the season of dust activity, particularly September to March. In contrast, background aerosol levels during May, June and July remained stable. The enhanced aerosol loadings during the latter 5 years of the study period can be understood as a combination of dune destabilisation through loss of ephemeral vegetation and surface crust, and the changing supply of fluvial sediments to ephemeral lakes and floodplains within the Lake Eyre Basin. Major dust outbreaks are generally highly localised, although significant dust activity was observed at Tinga Tingana on 50% of days when a major event occurred elsewhere in the Lake Eyre Basin, suggesting frequent basin-wide dust mobilisation. Combined analysis of aerosol optical depth and scattering coefficient shows weak correlation between the surface and column aerosol (R2=0.24). The aerosol scale height is broadly distributed with a mode typically between 2–3 km, with clearly defined seasonal variation. Climatological analysis reveals bimodal structure in the annual cycle of aerosol optical depth, with a summer peak related to maximal dust activity, and a spring peak related to lofted fine-mode aerosol. There is evidence for an increase in near-surface aerosol during the period 2003–2007 relative to 1997–2002, consistent with an increase in dust activity. This accords with an independent finding of increasing aerosol loading over the Australian region as a whole, suggesting that rising dust activity over the Lake Eyre Basin may be a significant contributor to changes in the aerosol budget of the continent.
Smoke injection heights from fires in North America: analysis of 5 years of satellite observations

We analyze an extensive record of aerosol smoke plume heights derived from observations over North America for the fire seasons of 2002 and 2004–2007 made by the Multi-angle Imaging SpectroRadiometer (MISR) instrument on board the NASA Earth Observing System Terra satellite. We characterize the magnitude and variability of smoke plume heights for various biomes, and assess the contribution of local atmospheric and fire conditions to this variability. Plume heights are highly variable, ranging from a few hundred meters up to 5000 m above the terrain at the Terra overpass time (11:00–14:00 local time). The largest plumes are found over the boreal region (median values of ~850 m height, 24 km length and 940 m thickness), whereas the smallest plumes are found over cropland and grassland fires in the contiguous US (median values of ~530 m height, 12 km length and 550–640 m thickness). The analysis of plume heights in combination with assimilated meteorological observations from the NASA Goddard Earth Observing System indicates that a significant fraction (4–12%) of plumes from fires are injected above the boundary layer (BL), consistent with earlier results for Alaska and the Yukon Territories during summer 2004. Most of the plumes located above the BL (>83%) are trapped within stable atmospheric layers. We find a correlation between plume height and the MODerate resolution Imaging Spectroradiometer (MODIS) fire radiative power (FRP) thermal anomalies associated with each plume. Smoke plumes located in the free troposphere (FT) exhibit larger FRP values (1620–1640 MW) than those remaining within the BL (174–465 MW). Plumes located in the FT without a stable layer reach higher altitudes and are more spread-out vertically than those associated with distinct stable layers (2490 m height and 2790 m thickness versus 1880 m height and 1800 m thickness). The MISR plume climatology exhibits a well-defined seasonal cycle of plume heights in boreal and temperate biomes, with greater heights during June–July. MODIS FRP measurements indicate that larger summertime heights are the result of higher fire intensity, likely due to more severe fire weather during these months. This work demonstrates the significant effect of fire intensity and atmospheric structure on the ultimate rise of fire emissions, and underlines the importance of considering such physical processes in modeling smoke dispersion.
Aerosol distribution around Svalbard during intense easterly winds

This paper reports on backscatter and depolarization measurements by an airborne lidar in the Arctic during the ASTAR 2004 campaign. A unique weather situation facilitated the observation of the aerosol concentration under strongly forced atmospheric conditions. The vigorous easterly winds distorted the flow past Svalbard in such a way that mesoscale features were visible in the remote-sensing observations: The formation of a well-mixed aerosol layer inside the Adventdalen and the subsequent thinning of the aerosol plume were observed over the Isfjorden. Additionally, mobilization of sea salt aerosols due to a coastal low-level jet at the northern tip of Svalbard resulted in a sloped boundary layer toward north. Mesoscale numerical modelling was applied to identify the sources of the aerosol particles and to explain the observed patterns.
Water-soluble SOA from Alkene ozonolysis: composition and droplet activation kinetics inferences from analysis of CCN activity

Cloud formation characteristics of the water-soluble organic fraction (WSOC) of secondary organic aerosol (SOA) formed from the ozonolysis of alkene hydrocarbons (terpinolene, 1-methlycycloheptene and cycloheptene) are studied. Based on size-resolved measurements of CCN activity (of the pure and salted WSOC samples) we estimate the average molar volume and surface tension depression associated with the WSOC using Köhler Theory Analysis (KTA). Consistent with known speciation, the results suggest that the WSOC are composed of low molecular weight species, with an effective molar mass below 200 g mol−1. The water-soluble carbon is also surface-active, depressing surface tension 10–15% from that of pure water (at CCN-relevant concentrations). The inherent hygroscopicity parameter, κ, of the WSOC ranges between 0.17 and 0.25; if surface tension depression and molar volume effects are considered in κ, a remarkably constant "apparent" hygroscopicity ~0.3 emerges for all samples considered. This implies that the volume fraction of soluble material in the parent aerosol is the key composition parameter required for prediction of the SOA hygroscopicity, as shifts in molar volume across samples are compensated by changes in surface tension. Finally, using "threshold droplet growth analysis", the water-soluble organics in all samples considered do not affect CCN activation kinetics.
Influences of in-cloud aerosol scavenging parameterizations on aerosol concentrations and wet deposition in ECHAM5-HAM

A diagnostic cloud nucleation scavenging scheme, which determines stratiform cloud scavenging ratios for both aerosol mass and number distributions, based on cloud droplet, and ice crystal number concentrations, is introduced into the ECHAM5-HAM global climate model. This scheme is coupled with a size-dependent in-cloud impaction scavenging parameterization for both cloud droplet-aerosol, and ice crystal-aerosol collisions. The aerosol mass scavenged in stratiform clouds is found to be primarily (>90%) scavenged by cloud nucleation processes for all aerosol species, except for dust (50%). The aerosol number scavenged is primarily (>90%) attributed to impaction. 99% of this impaction scavenging occurs in clouds with temperatures less than 273 K. Sensitivity studies are presented, which compare aerosol concentrations, burdens, and deposition for a variety of in-cloud scavenging approaches: prescribed fractions, a more computationally expensive prognostic aerosol cloud processing treatment, and the new diagnostic scheme, also with modified assumptions about in-cloud impaction and nucleation scavenging. Our results show that while uncertainties in the representation of in-cloud scavenging processes can lead to differences in the range of 20–30% for the predicted annual, global mean aerosol mass burdens, and near to 50% for accumulation mode aerosol number burden, the differences in predicted aerosol mass concentrations can be up to one order of magnitude, particularly for regions of the middle troposphere with temperatures below 273 K where mixed and ice phase clouds exist. Different parameterizations for impaction scavenging changed the predicted global, annual mean number removal attributed to ice clouds by seven-fold, and the global, annual dust mass removal attributed to impaction by two orders of magnitude. Closer agreement with observations of black carbon profiles from aircraft (increases near to one order of magnitude for mixed phase clouds), mid-troposphere 210Pb vertical profiles, and the geographic distribution of aerosol optical depth is found for the new diagnostic scavenging scheme compared to the prescribed scavenging fraction scheme of the standard ECHAM5-HAM. The diagnostic and prognostic schemes represent the variability of scavenged fractions particularly for submicron size aerosols, and for mixed and ice phase clouds, and are recommended in preference to the prescribed scavenging fractions method.
Atmospheric oxygen and carbon dioxide observations from two European coastal stations 2000–2005: continental influence, trend changes and APO climatology

Seeking for baseline conditions has biased the atmospheric carbon dioxide (CO2) and later on also oxygen (O2) monitoring networks towards remote marine stations, missing part of the variability that is due to regional anthropogenic as well as land biotic activity. We present here a five-year record of atmospheric CO2 concentrations and oxygen/nitrogen (O2/N2) ratio measurements from the coastal stations Lutjewad (LUT), The Netherlands and Mace Head (MHD), Ireland, derived from flask samples. O2/N2 ratios, a proxy for O2 concentrations, concurrently measured with CO2 concentrations, help determine regional CO2 fluxes by separating land fluxes from sea fluxes. Mace Head is the closest marine baseline station to Lutjewad, located at the same latitude, and therefore is taken as a reference. During the studied period, from 2000 until 2005, we observed an average increase of CO2 in the atmosphere of (1.7±0.2) ppm y−1, and a change of the O2/N2 ratio of (−20±1) per meg y−1. The difference between the CO2 summer minimum and the winter maximum is 14.4 ppm and 16.1 ppm at Mace Head and Lutjewad, respectively, while the paraphase variation in the O2 signal equals 113 per meg and 153 per meg, respectively. We also studied the atmospheric potential oxygen (APO) tracer at both stations. By this analysis, evidence has been found that we need to be careful when using APO close to anthropogenic CO2 sources. It could be biased by combustion-derived CO2, and models need to take into account daily and seasonal variations in the anthropogenic CO2 production in order to be able to simulate APO over the continents.
Results from the CERN pilot CLOUD experiment

During a 4-week run in October–November 2006, a pilot experiment was performed at the CERN Proton Synchrotron in preparation for the Cosmics Leaving OUtdoor Droplets (CLOUD) experiment, whose aim is to study the possible influence of cosmic rays on clouds. The purpose of the pilot experiment was firstly to carry out exploratory measurements of the effect of ionising particle radiation on aerosol formation from trace H2SO4 vapour and secondly to provide technical input for the CLOUD design. A total of 44 nucleation bursts were produced and recorded, with formation rates of particles above the 3 nm detection threshold of between 0.1 and 100 cm−3s−1, and growth rates between 2 and 37 nm h−1. The corresponding H2O concentrations were typically around 106 cm−3 or less. The experimentally-measured formation rates and H2SO4 concentrations are comparable to those found in the atmosphere, supporting the idea that sulphuric acid is involved in the nucleation of atmospheric aerosols. However, sulphuric acid alone is not able to explain the observed rapid growth rates, which suggests the presence of additional trace vapours in the aerosol chamber, whose identity is unknown. By analysing the charged fraction, a few of the aerosol bursts appear to have a contribution from ion-induced nucleation and ion-ion recombination to form neutral clusters. Some indications were also found for the accelerator beam timing and intensity to influence the aerosol particle formation rate at the highest experimental SO2 concentrations of 6 ppb, although none was found at lower concentrations. Overall, the exploratory measurements provide suggestive evidence for ion-induced nucleation or ion-ion recombination as sources of aerosol particles. However in order to quantify the conditions under which ion processes become significant, improvements are needed in controlling the experimental variables and in the reproducibility of the experiments. Finally, concerning technical aspects, the most important lessons for the CLOUD design include the stringent requirement of internal cleanliness of the aerosol chamber, as well as maintenance of extremely stable temperatures (variations below 0.1 °C
BVOC ecosystem flux measurements at a high latitude wetland site

In this study, we present summertime concentrations and fluxes of biogenic volatile organic compounds (BVOCs) measured at a sub-arctic wetland in northern Sweden using a disjunct eddy-covariance (DEC) technique based on a proton transfer reaction mass spectrometer (PTR-MS). The vegetation at the site was dominated by Sphagnum, Carex and extit{Eriophorum} spp. The measurements reported here cover a period of 50 days (1 August to 19 September 2006), approximately one half of the growing season at the site, and allowed to investigate the effect of day-to-day variation in weather as well as of vegetation senescence on daily BVOC fluxes, and on their temperature and light responses. The sensitivity drift of the DEC system was assessed by comparing H3O+-ion cluster formed with water molecules (H3O+(H2O) at m37) with water vapour concentration measurements made using an adjacent humidity sensor, and the applicability of the DEC method was analysed by a comparison of sensible heat fluxes for high frequency and DEC data obtained from the sonic anemometer. These analyses showed no significant PTR-MS sensor drift over a period of several weeks and only a small flux-loss due to high-frequency spectrum omissions. This loss was within the range expected from other studies and the theoretical considerations. Standardised (20 °C and 1000 μmol m−2 s−1 PAR) summer isoprene emission rates found in this study of 329 μg C m−2 (ground area) h−1 were comparable with findings from more southern boreal forests, and fen-like ecosystems. On a diel scale, measured fluxes indicated a stronger temperature dependence than emissions from temperate or (sub)tropical ecosystems. For the first time, to our knowledge, we report ecosystem methanol fluxes from a sub-arctic ecosystem. Maximum daytime emission fluxes were around 270 μg m−2 h−1 (ca. 100 μg C m−2 h−1), and during most nights small negative fluxes directed from the atmosphere to the surface were observed.