bluuebunny/crossref_metadata_2025 huggingface dataset:
Assessing the trends and effects of environmental parameters on the behavior of mercury in the lower atmosphere over cropped land over four seasons
Authors: Baya A. P. , van Heyst B.
Published: April 2010

Abstract. Mercury is released to the atmosphere from natural and anthropogenic sources. Due to its persistence in the atmosphere, mercury is subject to long range transport and is thus a pollutant of global concern. The terrestrial ecosystem is an important atmospheric mercury sink as a significant portion of the mercury emitted can be accumulated on soil surfaces making terrestrial surfaces an important source of previously emitted and deposited mercury. Studying the factors and processes that influence the behavior of mercury from terrestrial sources is thus important for a better understanding of the role of natural ecosystems in the mercury cycling and emission budget. A one year study (July 2006–August 2007) was conducted at Elora, Ontario, Canada to measure total gaseous mercury (TGM), reactive gaseous mercury (RGM) and particulate bound mercury (HgP) as well as TGM fluxes over different ground cover spanning the four seasons typical of a temperate climate zone. TGM concentrations were measured using a mercury vapour analyzer (Tekran 2537A) while RGM and HgP were measured with the Tekran 1130/1135 speciation unit coupled to another mercury vapour analyzer. A micrometeorological approach was used for TGM flux determination using a continuous two-level sampling system for TGM concentration gradient measurement above the soil surface and crop canopy. The turbulent transfer coefficients were derived from meteorological parameters measured on site. A net TGM volatilization (6.31±33.98 ng m−2 h−1, annual average) to the atmosphere was observed during the study. Average TGM concentrations and TGM fluxes showed significant seasonal differences and distinct diurnal patterns while no trends were observed for HgP or RGM. Highest TGM concentrations recorded in late spring and fall were due to meteorological changes such as increases in net radiation and air temperature in spring and lower atmospheric mixing height in fall. Highest TGM fluxes (18.1 ng m−2 h−1, monthly average) were recorded in late spring but also during specific events in winter and fall. The main factors influencing TGM flux were soil moisture content, soil temperature, precipitation events and ground cover. These trends indicate that the soil surface could be a significant mercury source in spring and summer seasons but also under specific meteorological conditions in winter or fall.
Long-term trends in the middle atmosphere dynamics at northern middle latitudes – one regime or two different regimes?
Authors: Lastovicka J. , Krizan P. , Kozubek M.
Published: April 2010

Abstract. Due to increasing atmospheric concentration of greenhouse gases and changing stratospheric ozone concentration, both of anthropogenic origin, various quantities in the middle atmosphere reveal long-term changes and trends. Lastovicka and Krizan (2006) indicated possibility of change of trends in the dynamics in the northern midlatitude middle atmosphere as a whole in the 1990s. To search for such change of trends we use data on winds in the mesopause region, on total columnar ozone, on ozone laminae, on winds in the middle and lower stratosphere, and on peak electron density in the E region of the ionosphere. One group of quantities, the mesopause region wind-like trends, changes their trends around 1990, the other one, the total ozone-like trends, in the mid-1990s. Altogether they create a skeleton of scenario of the change of the middle atmosphere dynamics trends in the 1990s. Drivers of these changes appear to be different for the first group and for the second group. Tropospheric processes seem to play a role in the changes of trends in middle atmospheric dynamics.
A case study of dust aerosol radiative properties over Lanzhou, China
Authors: Zhang L. , Cao X. , Bao J. , Zhou B. , Huang J. , Shi J. , Bi J.
Published: April 2010

Abstract. The vertical distribution of dust aerosol and its radiative properties are analysed using the data measured by the micropulse lidar, profiling microwave radiometer, sunphotometer, particulate monitor, and nephelometer at the Semi-Arid Climate and Environment Observatory of Lanzhou University (SACOL) during a dust storm from 27 March to 29 March 2007. The analysis shows that the dust aerosol mainly exists below 2 km in height, and the dust aerosol extinction coefficient decreases with height. The temporal evolution of aerosol optical depth (AOD) during the dust storm is characterized by a sub-maximum at 22:00 (Beijing Time) on 27 March and a maximum at 12:00 on 28 March. The AOD derived by lidar is compared with that obtained by sunphotometer, and shows a good consistency. The PM10 concentration and aerosol scattering coefficient share identical variation trends, and their maximums both appear at 22:00 on 27 March. The aerosol extinction coefficient and relative humidity have the same trends and their maximums appear at identical heights, showing a correlation between extinction coefficient and relative humidity known as aerosol hygroscopicity. Nevertheless, the correlation between aerosol extinction coefficient and temperature cannot be obviously seen. The aerosol extinction coefficient, scattering coefficient, and PM10 concentration present good linear correlations. The correlation coefficients of the aerosol scattering coefficient and PM10 concentration, of aerosol extinction coefficient and PM10 concentration, and of aerosol extinction and scattering coefficient are respectively 0.98, 0.94, and 0.96.
Insights into secondary organic aerosol formed via aqueous-phase reactions of phenolic compounds based on high resolution mass spectrometry
Authors: Sun Y. , Zhang Q. , Anastasio C. , Sun J.
Published: April 2010

Abstract. Recent work has shown that aqueous-phase reactions of phenolic compounds – phenol (C6H6O), guaiacol (C7H8O2), and syringol (C8H10O3) – can form secondary organic aerosol (SOA) at high yields. Here we examine the chemical characteristics of this SOA and its formation mechanisms using a High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-AMS), an Ion Chromatograph (IC), and a Total Organic Carbon (TOC) analyzer. The phenolic SOA are highly oxygenated with oxygen-to-carbon (O/C) ratios in the range of 0.80–1.06 and carbon oxidation states (=2×O/C–H/C) between −0.14 and +0.47. The organic mass-to-carbon (OM/OC) ratios determined by the HR-AMS (=2.21–2.55) agree well with values determined based on the SOA mass measured gravimetrically and the OC mass from the TOC analyzer. Both the O/C and OM/OC ratios of the phenolic SOA are similar to the values observed for ambient low-volatility oxygenated/secondary OA (LV-OOA). Oxalate is a minor, but ubiquitous, component of the SOA formed from all three phenolic precursors, accounting for 1.4–5.2% of the SOA mass, with generally higher yields in experiments with H2O2 added as an ·OH source compared to without. The AMS spectra show evidence for the formation of syringol and guaiacol dimers and higher oligomers via C–C and C–O coupling of phenoxyl radicals, which are formed through oxidation pathways such as abstraction of the phenolic hydrogen atom or ·OH addition to the aromatic ring. This latter pathway leads to hydroxylation of the aromatic ring, which is one mechanism that increases the degree of oxidation of the SOA products. Compared to direct photochemical reactions of the phenols, ·OH-initiated reactions favor the formation of smaller oxidation products but less dimers or higher oligomers. Two unique and prominent ions in the syringol and guaiacol SOA spectra, m/z 306 (C16H18O6+) and m/z 246 (C14H14O4+), respectively, are observed in ambient aerosols significantly influenced by wood combustion and fog processing. Our results indicate that cloud and fog processing of phenolic compounds, especially in areas with active biomass burning, might represent an important pathway for the formation of low-volatility and highly oxygenated organic species, which would remain in particle phase after fog/cloud evaporation and affect the hygroscopicity and radiative impacts of ambient OA.
Analysis of emission data from global commercial aviation: 2004 and 2006
Authors: Wilkerson J. T. , Jacobson M. Z. , Malwitz A. , Balasubramanian S. , Wayson R. , Fleming G. , Naiman A. D. , Lele S. K.
Published: April 2010

Abstract. The global commercial aircraft fleet in 2006 flew more than 31 million flights, burned nearly 190 million metric tons of fuel, and covered 38 billion kilometers. This activity emitted substantial amounts of fossil-fuel combustion products within the upper troposphere and lower stratosphere that affect atmospheric composition and climate. The emissions products, such as carbon monoxide, carbon dioxide, oxides of nitrogen, sulfur compounds, and particulate matter, are not emitted uniformly over the Earth, so understanding the temporal and spatial distributions is an important component for modeling aviation climate impacts. Here, we analyze global commercial aircraft emission data for 2004 and 2006. Data, provided by the Volpe National Transportation Systems Center, were computed using the Federal Aviation Administration's Aviation Environmental Design Tool. For both years, analysis of flight data shows 93 percent of fuel was burned in the Northern Hemisphere, 69 percent between 30 N and 60 N latitudes; 77 (75) percent was burned above 7 km in 2004 (2006). This activity led to 177 (162) Tg of carbon from CO2 globally in 2004 (2006), with half being emitted over three dominant regions: United States, Europe, East Asia. The difference between 2004 and 2006 is a result of fewer flights in 2006 and the methodology used to compute fuel burn and emissions from those flights. We also show that despite receiving only a few percent of global emissions, the Arctic receives a concentration of emissions of the same order of magnitude as the global average. The following is a summary of this data which illustrates the global and regional aviation emissions footprints for 2004 and 2006, and provides temporal and spatial distribution statistics of several emissions constituents. Finally, we show that 87 (85) percent of all flights in 2004 (2006) are short-haul missions, yet those flights are responsible for only 38 (39) percent of total emissions.
Observations of turbulence-induced new particle formation in the residual layer
Authors: Wehner B. , Siebert H. , Ansmann A. , Ditas F. , Seifert P. , Stratmann F. , Wiedensohler A. , Apituley A. , Shaw R. A. , Manninen H. E. , Kulmala M.
Published: April 2010

Abstract. Aerosol particle measurements in the atmospheric boundary layer performed by a helicopter-borne measurement payload and by a lidar system from a case study during the IMPACT field campaign in Cabauw (NL) are presented. Layers of increased number concentrations of ultrafine particles were observed in the residual layer, indicating relatively recent new-particle formation. These layers were characterized by a sub-critical Richardson number and concomitant increased turbulence. Turbulent mixing is likely to lead to local supersaturation of possible precursor gases which are essential for new particle formation. Observed peaks in the number concentrations of ultrafine particles at ground level are connected to the new particle formation in the residual layer by boundary layer development and vertical mixing.
A comparison of ship and satellite measurements of cloud properties in the southeast Pacific stratus deck
Authors: Brunke M. A. , de Szoeke S. P. , Zuidema P. , Zeng X.
Published: April 2010

Abstract. Here, liquid water path (LWP), cloud fraction, cloud top height, and cloud base height are retrieved by a suite of satellite instruments (the CPR aboard CloudSat, CALIOP aboard CALIPSO, and MODIS aboard Aqua) and compared to ship observations from research cruises made in 2001 and 2003–2007 into the stratus/stratocumulus deck over the southeast Pacific Ocean. It is found that CloudSat LWP is generally too high over this region and the CloudSat/CALIPSO cloud bases are too low which is to be expected from the increased sensitivity to precipitation by both the radar and lidar. This results in a relationship (LWP~h9) between CloudSat LWP and CALIPSO cloud thickness (h) that is very different from the adiabatic relationship (LWP~h2) from in situ observations. Furthermore, comparing results from a global model (CAM3.1) to ship observations reveals that, while the simulated LWP is quite reasonable, the model cloud is too thick and too low, allowing the model to have LWPs that are almost independent of h. Such differences may be reduced in future versions of both the satellite data and the model.
Measurements and receptor modeling of volatile organic compounds in south-eastern Mexico City, 2000–2007
Authors: Wöhrnschimmel H. , Magaña M. , Stahel W. A. , Blanco S. , Acuña S. , Pérez J. M. , González S. , Gutiérrez V. , Wakamatsu S. , Cárdenas B.
Published: April 2010

Abstract. Ambient samples of volatile organic compounds (VOCs) were measured between 2000 and 2007 in south-eastern Mexico City, quantifying 13 species (ethane, propane, propylene, butane, acetylene, pentane, hexane, heptane, benzene, octane, toluene, nonane, o-xylene). These time series were analyzed for long-term trends, using linear regression models. A main finding was that the concentrations for several of the quantified VOC species were decreasing during this period. A receptor model was applied to identify possible VOC sources, as well as temporal patterns in their respective activities. Domestic use of liquefied petroleum gas and vehicle exhaust are suggested to be the principal emission sources, contributing together between 70% and 80% to total VOC. Both diurnal and seasonal patterns, as well as a weekend effect were recognized in the modelled source activities. Furthermore, vehicle exhaust emissions showed a decreasing trend over time, with a reduction of about 8% per year.
CO2 column-averaged volume mixing ratio derived over Tsukuba from measurements by commercial airlines
Authors: Araki M. , Morino I. , Machida T. , Sawa Y. , Matsueda H. , Yokota T. , Uchino O.
Published: April 2010

Abstract. Column-averaged volume mixing ratios of carbon dioxide (XCO2) during the period from January 2007 to May 2008 over Tsukuba, Japan, were derived by using CO2 concentration data observed by Japan Airlines Corporation (JAL) commercial airliners, based on the assumption that CO2 profiles over Tsukuba and Narita were the same. CO2 profile data for 493 flights on clear-sky days were analysed in order to calculate XCO2 with an ancillary dataset: Tsukuba observational data (by rawinsonde and a meteorological tower) or global meteorological data (NCEP and CIRA-86). The amplitude of seasonal variation of XCO2 (Tsukuba observational) from the Tsukuba observational data was determined by least-squares fit using a harmonic function to roughly evaluate the seasonal variation over Tsukuba. The highest and lowest values of the obtained fitted curve in 2007 for XCO2 (Tsukuba observational) were 386.4 and 381.7 ppm in May and September, respectively. The dependence of XCO2 on the type of ancillary dataset was evaluated. The average difference between XCO2 (global) from global climatological data and XCO2 (Tsukuba observational), i.e., the bias of XCO2 (global) based on XCO2 (Tsukuba observational), was found to be -0.621 ppm with a standard deviation of 0.682 ppm. The uncertainty of XCO2 (global) based on XCO2 (Tsukuba observational) was estimated to be 0.922 ppm. This small uncertainty suggests that the present method of XCO2 calculation using data from airliners and global climatological data can be applied to the validation of GOSAT products for XCO2 over airports worldwide.
Investigation of the correlation between odd oxygen and secondary organic aerosol in Mexico City and Houston
Authors: Wood E. C. , Canagaratna M. R. , Herndon S. C. , Kroll J. H. , Onasch T. B. , Kolb C. E. , Worsnop D. R. , Knighton W. B. , Seila R. , Zavala M. , Molina L. T. , DeCarlo P. F. , Jimenez J. L. , Weinheimer A. J. , Knapp D. J. , Jobson B. T. , Stutz J. , Kuster W. C. , Williams E. J.
Published: April 2010

Abstract. Many recent models underpredict secondary organic aerosol (SOA) particulate matter (PM) concentrations in polluted regions, indicating serious deficiencies in the models' chemical mechanisms and/or missing SOA precursors. Since tropospheric photochemical ozone production is much better understood, we investigate the correlation of odd-oxygen ([Ox]≡[O3]+[NO2]) and the oxygenated component of organic aerosol (OOA), which is interpreted as a surrogate for SOA. OOA and Ox measured in Mexico City in 2006 and Houston in 2000 were well correlated in air masses where both species were formed on similar timescales (less than 8 h) and not well correlated when their formation timescales or location differed greatly. When correlated, the ratio of these two species ranged from 30 μg m−3 ppm−1 (STP) in Houston during time periods affected by large petrochemical plant emissions to as high as 160 μg m−3 ppm−1 in Mexico City, where typical values were near 120 μg m−3 ppm−1. On several days in Mexico City, the [OOA]/[Ox] ratio decreased by a factor of ~2 between 08:00 and 13:00 LT. This decrease is only partially attributable to evaporation of the least oxidized and most volatile components of OOA; differences in the diurnal emission trends and timescales for photochemical processing of SOA precursors compared to ozone precursors also likely contribute to the observed decrease. The extent of OOA oxidation increased with photochemical aging. Calculations of the ratio of the SOA formation rate to the Ox production rate using ambient VOC measurements and traditional laboratory SOA yields are lower than the observed [OOA]/[Ox] ratios by factors of 5 to 15, consistent with several other models' underestimates of SOA. Calculations of this ratio using emission factors for organic compounds from gasoline and diesel exhaust do not reproduce the observed ratio. Although not succesful in reproducing the atmospheric observations presented, modeling P(SOA)/P(Ox) can serve as a useful test of photochemical models using improved formulation mechanisms for SOA.
The invigoration of deep convective clouds over the Atlantic: aerosol effect, meteorology or retrieval artifact?
Authors: Koren I. , Feingold G. , Remer L. A.
Published: April 2010

Abstract. The effects of the aerosol on convective clouds in the tropical Atlantic Ocean are explored using satellite remote sensing, a chemical transport model, and a reanalysis of meteorological fields. Two of the most challenging problems are addressed: the potential for elements of the cloud field to be erroneously ascribed to aerosol optical depth; and the potential for correlations between aerosol and cloud parameters to be erroneously considered to be causal. Results show that there is a robust positive correlation between cloud fraction or cloud top height and the aerosol optical depth, regardless of whether a stringent filtering of aerosol measurements in the vicinity of clouds is applied, or not. These same positive correlations emerge when replacing the observed aerosol field with that derived from a chemical transport model. A correlation exercise between the full suite of meteorological fields derived from model reanalysis and satellite-derived cloud fields shows that observed cloud top height and cloud fraction correlate best with pressure updraft velocity and relative humidity. Observed aerosol optical depth does correlate with meteorological parameters but usually different parameters from those that correlate with observed cloud fields. The result is a near-orthogonal influence of aerosol and meteorological fields on cloud top height and cloud fraction. The results strengthen the case that the aerosol does play a role in invigorating convective clouds.
Heterogeneous chemistry of monocarboxylic acids on α-Al2O3 at ambient condition
Authors: Tong S. R. , Wu L. Y. , Ge M. F. , Wang W. G. , Pu Z. F.
Published: April 2010

Abstract. A study of the atmospheric heterogeneous reactions of formic acid, acetic acid, and propionic acid on dust particles (α-Al2O3) was performed at ambient condition by using a diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) reactor. From the analysis of the spectral features, observations of carboxylates formation provide strong evidence for an efficient reactive uptake process. Comparison of the calculated and experimental vibrational frequencies of adsorbed carboxylates establishes the bridging coordinated structures on the surface. The uptake coefficients of formic acid, acetic acid, and propionic acid on α-Al2O3 particles are (2.07±0.26)×10−3, (5.00±0.69)×10−3, and (3.04±0.63)×10−3, respectively (using geometric area). Besides, the effect of various relative humid (RH) on this heterogeneous reactions was studied. The uptake coefficients of monocarboxylic acids on α-Al2O3 particles increase initially (RH<20%) and then decrease with the increased RH (RH>20%) which was due to the effect of water on carboxylic acids solvation, particles surface hydroxylation, and competition on reactive site. On the basis of the results of experimental simulation, the mechanism of heterogeneous reaction of dust with carboxylic acids at ambient condition was discussed. The loss of atmospheric monocarboxylic acids due to reactive uptake on available mineral dust particles can be competitive with homogeneous loss pathways, especially in dusty urban and desertified environments.
Water vapor budget associated to overshoots in the tropical stratosphere: mesoscale modelling study of 4–5 August 2006 during SCOUT-AMMA
Authors: Liu X. M. , Rivière E. D. , Marécal V. , Durry G. , Hamdouni A. , Arteta J. , Khaykin S.
Published: April 2010

Abstract. The aim of this paper is to study the impacts of overshooting convection at a local scale on the water distribution in the tropical UTLS. Overshooting convection is likely to be one of the key processes controlling the entry of water vapour amount in the stratosphere by injecting ice crystals above the tropopause which later sublimate and hydrate the lower stratosphere. For this purpose, we quantify the individual impact of two overshooting cases in Africa observed during SCOUT-AMMA: the case of 4 August 2006 over Southern Chad which is likely to have influenced the water vapour measurements by micro-SDLA and FLASH-B from Niamey on 5 August, and the case of a mesoscale convective system over Aϊr on 5 August 2006. We make use of high resolution (down to 1 km horizontally) three nested grid simulations with the three-dimensional regional atmospheric model BRAMS (Brazilian Regional Atmospheric Modelling System). In both cases, BRAMS succeeds in simulating the main features of the convective activity, as well as overshooting convection, thought the exact position and time of the overshoots indicated by MSG brightness temperature difference is not fully reproduced (typically 1° in latitude compared with the overshoots indicated by brightness temperature difference from satellite observations for both cases, and several hours shift the Aϊr case on 5 August 2006). Total water budgets associated with these two events show a significant injection of ice particles above the tropopause with maximum values of about 3.7 ton s−1 for the Chad case (4 August) and 1.4 ton s−1 for the Aϊr case (5 August), and a total cross tropopause transport of about 3300 ton h−1 for the Chad case and 2400 ton h−1 for the Aϊr case in the third domain of simulation. The order of magnitude of these modelled fluxes is lower but comparable with similar studies in other tropical areas based on models. These two estimations exhibit significant differences and highlight variability among the cases of the impact of overshooting convection in hydrating the lower stratosphere. We show that the regional enhancement of water above the tropopause is between 0.21 to 0.67 ppmv between 380 K and 400 K, in the range of other model estimations. Finally we emphasize that as long as the model resolution is high, the hydrated area in the LS by overshooting convection can be advected relatively far away from the overshoot initial location, with locally mixing ratios of more than 3 ppmv higher than the background level, which is compatible with the balloon borne measurements performed above Niamey in the same air mass, 30 h after the overshoot. However, in the model, when exiting the highest resolution grid, the hydrating signal is lost rapidly.
The potential influence of Asian and African mineral dust on ice, mixed-phase and liquid water clouds
Authors: Wiacek A. , Peter T. , Lohmann U.
Published: April 2010

Abstract. This modelling study explores the availability of mineral dust particles as ice nuclei for interactions with ice, mixed-phase and liquid water clouds, also tracking the particles' history of cloud-processing. We performed 61 320 one-week forward trajectory calculations originating near the surface of major dust emitting regions in Africa and Asia using high-resolution meteorological analysis fields for the year 2007. Without explicitly modelling dust emission and deposition processes, dust-bearing trajectories were assumed to be those coinciding with known dust emission seasons. We found that dust emissions from Asian deserts lead to a higher potential for interactions with high clouds, despite being the climatologically much smaller dust emission source. This is due to Asian regions experiencing significantly more ascent than African regions, with strongest ascent in the Asian Taklimakan desert at ~25%, ~40% and 10% of trajectories ascending to 300 hPa in spring, summer and fall, respectively. The specific humidity at each trajectory's starting point was transported in a Lagrangian manner and relative humidities with respect to water and ice were calculated in 6-h steps downstream, allowing us to estimate the formation of liquid, mixed-phase and ice clouds. Practically none of the simulated air parcels reached regions where homogeneous ice nucleation can take place (T≲−40 °C) along trajectories that have not experienced water saturation first. By far the largest fraction of cloud forming trajectories entered conditions of mixed-phase clouds, where mineral dust will potentially exert the biggest influence. The majority of trajectories also passed through regions supersaturated with respect to ice but subsaturated with respect to water, where "warm" (T≳−40 °C) ice clouds may form prior to supercooled water or mixed-phase clouds. The importance of "warm" ice clouds and the general influence of dust in the mixed-phase cloud region are highly uncertain due to considerable scatter in recent laboratory data from ice nucleation experiments, which we briefly review in this work. For "classical" cirrus-forming temperatures, our results show that only mineral dust IN that underwent mixed-phase cloud-processing previously are likely to be relevant, and, therefore, we recommend further systematic studies of immersion mode ice nucleation on mineral dust suspended in atmospherically relevant coatings.
Thunderstorm and stratocumulus: how does their contrasting morphology affect their interactions with aerosols?
Authors: Lee S. S. , Donner L. J. , Penner J. E.
Published: April 2010

Abstract. It is well-known that aerosols affect clouds and that the effect of aerosols on clouds is critical for understanding human-induced climate change. Most climate model studies have focused on the effect of aerosols on warm stratiform clouds (e.g., stratocumulus clouds) for the prediction of climate change. However, systems like the Asian and Indian Monsoon, storm tracks, and the intertropical convergence zone, play important roles in the global hydrological cycle and in the circulation of energy and are driven by thunderstorm-type convective clouds. Here, we show that the different morphologies of these two cloud types lead to different aerosol-cloud interactions. Increasing aerosols are known to suppress the conversion of droplets to rain (i.e., so-called autoconversion). This increases droplets as a source of evaporative cooling, leading to an increased intensity of downdrafts. The acceleration of the intensity of downdrafts is larger in convective clouds due to their larger cloud depths (providing longer paths for downdrafts to follow to the surface) than in stratiform clouds. More accelerated downdrafts intensify the gust front, leading to significantly increased updrafts, condensation and thus the collection of cloud liquid by precipitation, which offsets the suppressed autoconversion. This leads to an enhancement of precipitation with increased aerosols in convective clouds. However, the downdrafts are less accelerated in stratiform clouds due to their smaller cloud depths, and they are not able to induce changes in updrafts as large as those in convective clouds. Thus, the offset is not as effective, and this allows the suppression of precipitation with increased aerosols. Thus aerosols affect these cloud systems differently. The dependence of the effect of aerosols on clouds on the morphology of clouds should be taken into account for a more complete assessment of climate change.
Amine exchange into ammonium bisulfate and ammonium nitrate nuclei
Authors: Bzdek B. R. , Ridge D. P. , Johnston M. V.
Published: April 2010

Abstract. The exchange kinetics and thermodynamics of amines for ammonia in small (1–2 nm diameter) ammonium bisulfate and ammonium nitrate clusters were investigated using electrospray ionization Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR-MS). Ammonium salt clusters were reacted with amine gas at constant pressure to determine the kinetics of exchange. The reverse reactions, where aminium salt clusters reacted with ammonia gas, were also studied, and no substitution of ammonia for amine was observed. Gibbs free energy changes for these substitutions were determined to be highly exothermic, −7 kJ/mol or more negative in all cases. Uptake coefficients (reaction probabilities) were found to be near unity, implying that complete exchange of ammonia in small salt clusters by amine would be expected to occur within several seconds to minutes in the ambient atmosphere. These results suggest that if salt clusters are a component of the sub-3 nm cluster pool, they are likely to be aminium salts rather than ammonium salts, even if they were initially formed as ammonium salts.
Size-dependent aerosol deposition velocities during BEARPEX'07
Authors: Vong R. J. , Vong I. J. , Vickers D. , Covert D. S.
Published: April 2010

Abstract. Aerosol concentrations and 3-D winds were measured from 9 to 25 September 2007 above a pine forest in California. The measurements were combined using the eddy covariance (EC) technique to determine aerosol eddy fluxes as a function of particle diameter within the accumulation mode size range (0.25 μm< dia <1μm here). Measured heat and water vapor fluxes were utilized to correct the aerosol eddy fluxes for aerosol hygroscopic growth. The hygroscopic growth correction was necessary despite the low RH and relatively hygrophobic nature of the particles. Uncertainties associated with particle counting also were evaluated from the data. Aerosol deposition velocities (Vd = EC turbulent flux/mean particle concentration) during daytime were shown to vary from −0.2 to −1.0 cm s−1; |Vd| increases with friction velocity and particle diameter.
Long range transport of mercury to the Arctic and across Canada
Authors: Durnford D. , Dastoor A. , Figueras-Nieto D. , Ryjkov A.
Published: April 2010

Abstract. This study is the most extensive study to date on the transport of mercury to the Arctic. Moreover, it is the first such study to use a fully-coupled, online chemical transport model, Environment Canada's Global/Regional Atmospheric Heavy Metals model (GRAHM), where the meteorology and mercury processes are fully integrated. It is also the only study to date on the transport of mercury across Canada. We determined source attribution from Asia, North America, Russia and Europe at six arctic verification stations, as well as three subarctic and eight midlatitude Canadian stations. We have found that Asia, despite having transport efficiencies that were almost always lower than those of North America and often lower than those of Russia, was the dominant source of gaseous atmospheric mercury at all verification stations: it contributed the most mercury (29–37% at all stations, seasons and levels considered), its concentrations frequently explained nearly 100% of the variability in the concentrations produced by the simulation performed with full global emissions, particularly in the absence of local sources, and it generated the most long range transport (LRT) events, causing 43%, 67% and 75% of the events at the arctic, subarctic and midlatitude stations, respectively. For the Arctic, Russian transport efficiencies tended to be the strongest, as expected, while European and Asian efficiencies were lower and higher, respectively, than those found in the literature. This disagreement is likely produced by mercury's long lifetime relative to that of other pollutants. The accepted springtime preference for the trans-Pacific transport of Asian pollution was evident only in the midlatitude group of stations, being masked in the arctic and subarctic groups by the occurrence of atmospheric mercury depletion events. Some neighbouring arctic stations recorded dissimilar numbers of LRT events; despite their proximity, the behaviour of mercury at these stations was governed by different dynamics and transport pathways. The column burden of GEM in the lowest 5 km of the Northern Hemisphere was largest in summer from Asia, North America and Russia, but in winter from Europe. In the vertical, transport of mercury from all source regions occurred principally in the mid-troposphere.
Global mercury emissions to the atmosphere from anthropogenic and natural sources
Authors: Pirrone N. , Cinnirella S. , Feng X. , Finkelman R. B. , Friedli H. R. , Leaner J. , Mason R. , Mukherjee A. B. , Stracher G. B. , Streets D. G. , Telmer K.
Published: April 2010

Abstract. This paper provides an up-to-date assessment of global mercury emissions from anthropogenic and natural sources. On an annual basis, natural sources account for 5207 Mg of mercury released to the global atmosphere, including the contribution from re-emission processes, which are emissions of previously deposited mercury originating from anthropogenic and natural sources, and primary emissions from natural reservoirs. Anthropogenic sources, which include a large number of industrial point sources, are estimated to account for 2320 Mg of mercury emitted annually. The major contributions are from fossil-fuel fired power plants (810 Mg yr−1), artisanal small scale gold mining (400 Mg yr−1), non-ferrous metals manufacturing (310 Mg yr−1), cement production (236 Mg yr−1), waste disposal (187 Mg yr−1) and caustic soda production (163 Mg yr−1). Therefore, our current estimate of global mercury emissions suggests that the overall contribution from natural sources (primary emissions+re-emissions) and anthropogenic sources is nearly 7527 Mg per year, the uncertainty associated with these estimates are related to the typology of emission sources and source regions.
Impact of deep convection in the tropical tropopause layer in West Africa: in-situ observations and mesoscale modelling
Authors: Fierli F. , Orlandi E. , Law K. S. , Cagnazzo C. , Cairo F. , Schiller C. , Borrmann S. , Didonfrancesco G. , Ravegnani F. , Volk M.
Published: April 2010

Abstract. We present the analysis of the impact of convection on the composition of the tropical tropopause layer region (TTL) in West-Africa during the AMMA-SCOUT campaign. Geophysica M55 aircraft observations of water vapor, ozone, aerosol and CO2 show perturbed values at altitudes ranging from 14 km to 17 km (above the main convective outflow) and satellite data indicates that air detrainment is likely originated from convective cloud east of the flight. Simulations of the BOLAM mesoscale model, nudged with infrared radiance temperatures, are used to estimate the convective impact in the upper troposphere and to assess the fraction of air processed by convection. The analysis shows that BOLAM correctly reproduces the location and the vertical structure of convective outflow. Model-aided analysis indicates that in the outflow of a large convective system, deep convection can largely modify chemical composition and aerosol distribution up to the tropical tropopause. Model analysis also shows that, on average, deep convection occurring in the entire Sahelian transect (up to 2000 km E of the measurement area) has a non negligible role in determining TTL composition.
Transport of dust particles from the Bodélé region to the monsoon layer: AMMA case study of the 9–14 June 2006 period
Authors: Crumeyrolle S. , Tulet P. , Garcia-Carreras L. , Flamant C. , Parker D. J. , Matsuki A. , Schwarzenboeck A. , Formenti P. , Gomes L.
Published: April 2010

Abstract. Aerosol properties were measured during an airborne campaign experiment that took place in June 2006 in West Africa within the framework of the African Monsoon Multidisciplinary Analyses (AMMA). The goal of the present study was to determine the process that facilitates the sedimentation of dust particles from the Saharan Air Layer (SAL) to the boundary layer. A significant change in the dust particle concentration measured along the meridian between Niamey (Niger) and Cotonou (Benin) was found in the boundary layer (~700 m), where the dust particle concentration increased in a zone where local emission is not possible. Moreover, the boundary layer top observed with the dropsondes launched with the F-F20 shows a strong relationship with the surface cover anomalies, with higher Boundary Layer (BL) tops over the warmer surfaces, such as croplands, as opposed to adjacent forest. A mesoscale atmospheric model with a new on-line dust parameterization, resulting from the Alfaro and Gomes (2001) parametrisation and AMMA observations, was used to interpret the impact of vegetation anomalies on dust particle sedimentation. The results of the simulation are consistent with the observations, with higher dust over the warm surface cover anomalies.
Development and application of a reactive plume-in-grid model: evaluation over Greater Paris
Authors: Korsakissok I. , Mallet V.
Published: April 2010

Abstract. Emissions from major point sources are badly represented by classical Eulerian models. An overestimation of the horizontal plume dilution, a bad representation of the vertical diffusion as well as an incorrect estimate of the chemical reaction rates are the main limitations of such models in the vicinity of major point sources. The plume-in-grid method is a multiscale modeling technique that couples a local-scale Gaussian puff model with an Eulerian model in order to better represent these emissions. We present the plume-in-grid model developed in the air quality modeling system Polyphemus, with full gaseous chemistry. The model is evaluated on the metropolitan Île-de-France region, during six months (summer 2001). The subgrid-scale treatment is used for 89 major point sources, a selection based on the emission rates of NOx and SO2. Results with and without the subgrid treatment of point emissions are compared, and their performance by comparison to the observations at measurement stations is assessed. A sensitivity study is also carried out, on several local-scale parameters as well as on the vertical diffusion within the urban area. Primary pollutants are shown to be the most impacted by the plume-in-grid treatment, with a decrease in RMSE by up to about -17% for SO2 and -7% for NO at measurement stations. SO2 is the most impacted pollutant, since the point sources account for an important part of the total SO2 emissions, whereas NOx emissions are mostly due to traffic. The spatial impact of the subgrid treatment is localized in the vicinity of the sources, especially for reactive species (NOx and O3). Reactive species are mostly sensitive to the local-scale parameters, such as the time step between two puff emissions which influences the in-plume chemical reactions, whereas the almost-passive species SO2 is more sensitive to the injection time, which determines the duration of the subgrid-scale treatment. Future developments include an extension to handle aerosol chemistry, and an application to the modeling of line sources in order to use the subgrid treatment with road emissions. The latter is expected to lead to more striking results, due to the importance of traffic emissions for the pollutants of interest.
Variation of ambient non-methane hydrocarbons in Beijing city in summer 2008
Authors: Wang B. , Shao M. , Lu S. H. , Yuan B. , Zhao Y. , Wang M. , Zhang S. Q. , Wu D.
Published: April 2010

Abstract. In conjunction with hosting the 2008 Beijing Olympics, the municipal government implemented a series of stringent air quality control measures. To assess the impacts on variation of ambient non-methane hydrocarbons (NMHCs), the whole air was sampled by canisters at one urban site and two suburban sites in Beijing, and 55 NMHC species were quantified by gas chromatography equipped with a quadrupole mass spectrometer and a flame ionization detector (GC/MSD/FID) as parts of the field Campaign for the Beijing Olympic Games Air Quality program (CareBeijing). According to the control measures, the data were presented according to four periods: 18–30 June, 8–19 July, 15–24 August (during the Olympic Games), and 6–15 September (during the Paralympic Games). Compared with the levels in June, the mixing ratios of NMHCs obtained in the Olympic and Paralympic Games periods were reduced by 35% and 25%, respectively. Source contributions were calculated using a chemical mass balance model (CMB 8.2). After implementing the control measures, emissions from target sources were obviously reduced, and reductions in vehicle exhaust could explain 48–82% of the reductions of ambient NMHCs. Reductions in emissions from gasoline evaporation, paint and solvent use, and the chemical industry contributed 9–40%, 3–24%, and 1–5%, respectively, to reductions of ambient NMHCs. Sources of liquefied petroleum gas (LPG) and biogenic emissions were not controlled, and contributions from these sources from July to September were stable or even higher than in June. Ozone formation potentials (OFPs) were calculated for the measured NMHCs. The total OFPs during the Olympic and Paralympic Games were reduced by 48% and 32%, respectively, compared with values in June. Reductions in the OFPs of alkenes and aromatics explained 77–92% of total OFP reductions. The alkenes and aromatics were mainly from vehicle exhausts, and reductions of vehicle exhaust gases explained 67–87% of reductions in alkenes and 38–80% of reductions in aromatics. These findings demonstrate the effectiveness of the air quality control measures enacted for the 2008 Olympics and indicate that controlling vehicular emissions could be the most important measure to improve air quality in Beijing.
Aerosol optical properties and radiative forcing in the high Himalaya based on measurements at the Nepal Climate Observatory – pyramid site (5100 m a.s.l)
Authors: Marcq S. , Laj P. , Roger J. C. , Villani P. , Sellegri K. , Bonasoni P. , Marinoni A. , Cristofanelli P. , Verza G. P. , Bergin M.
Published: April 2010

Abstract. Intense anthropogenic emissions over the Indian sub-continent lead to the formation of layers of particulate pollution that can be transported to the high altitude regions of the Himalaya-Hindu-Kush (HKH). Aerosol particles contain a substantial fraction of strongly absorbing material, including black carbon (BC), organic compounds (OC), and dust all of which can contribute to atmospheric warming, in addition to greenhouse gases. Using a 3-year record of continuous measurements of aerosol optical properties, we present a time series of key climate relevant aerosol properties including the aerosol absorption (σap) and scattering (σsp) coefficients as well as the single-scattering albedo (w). Results of this investigation show substantial seasonal variability of these properties, with long range transport during the pre- and post-monsoon seasons and efficient precipitation scavenging of aerosol particles during the monsoon season. The monthly averaged scattering coefficients range from 0.1 Mm−1 (monsoon) to 20 Mm−1 while the average absorption coefficients range from 0.5 Mm−1 to 3.5 Mm−1. Both have their maximum values during the pre-monsoon period (April) and reach a minimum during Monsoon (July–August). This leads to w values from 0.86 (pre-monsoon) to 0.79 (monsoon) seasons. Significant diurnal variability due to valley wind circulation is also reported. Using typical air mass trajectories encountered at the station, and aerosol optical depth (aod) measurements, we calculated the resulting direct local radiative forcing due to aerosols. We found that the presence of absorbing particulate material can locally induce an additional top of the atmosphere (TOA) forcing of 10 to 20 W m−2 for the first atmospheric layer (500 m above surface). The TOA positive forcing depends on the presence of snow at the surface, and takes place preferentially during episodes of regional pollution occurring on a very regular basis in the Himalayan valleys. Warming of the first atmospheric layer is paralleled by a substantial decrease of the amount of radiation reaching the surface. The surface forcing is estimated to range from −4 to −20 W m−2 for small-scale regional pollution events and large-scale pollution events, respectively. The calculated surface forcing is also very dependent on surface albedo, with maximum values occurring over a snow-covered surface. Overall, this work presents the first estimates of aerosol direct radiative forcing over the high Himalaya based on in-situ aerosol measurements, and results suggest a TOA forcing significantly greater than the IPCC reported values for green house gases.
Tropospheric aerosol size distributions simulated by three online global aerosol models using the M7 microphysics module
Authors: Zhang K. , Wan H. , Wang B. , Zhang M. , Feichter J. , Liu X.
Published: April 2010

Abstract. Tropospheric aerosol size distributions are simulated by three online global models that employ exactly the same modal approach but differ in many aspects such as model meteorology, natural aerosol emissions, sulfur chemistry, and the parameterization of deposition processes. The main purpose of this study is to identify where the largest inter-model discrepancies occur and what the main reasons are. The number concentrations of different aerosol size ranges are compared among the three models and against observations. Overall all the three models can capture the basic features of the observed aerosol number spatial distributions. The magnitude of the number concentration of each mode is consistent among the three models. Quantitative differences are also clearly detectable. For the soluble and insoluble coarse mode and accumulation mode, inter-model discrepancies mainly result from differences in the sea salt and dust emissions, as well as the different strengths of the convective transport in the meteorological models. For the nucleation mode and the soluble Aitken mode, the spread of the model results is largest in the tropics and in the middle and upper troposphere. Diagnostics and sensitivity experiments suggest that this large spread is closely related to the sulfur cycle in the models, which is strongly affected by the choice of sulfur chemistry scheme, its coupling with the convective transport and wet deposition calculation, and the related meteorological fields such as cloud cover, cloud water content, and precipitation. The aerosol size distributions simulated by the three models are compared to observations in the boundary layer. The characteristic shape and magnitude of the distribution functions are reasonably reproduced in typical conditions (i.e., clean, polluted and transition areas). Biases in the mode parameters over the remote oceans and the China adjacent seas are probably caused by the fixed mode variance in the mathematical formulations used in the modal approach in the three models, as well as some of the prescribed size distribution parameters of the natural and anthropogenic emissions.