bluuebunny/crossref_metadata_2025 huggingface dataset:
Increasing synoptic scale variability in atmospheric CO2 at Hateruma Island associated with increasing East Asian emissions
Authors: Tohjima Y. , Mukai H. , Hashimoto S. , Patra P. K.
Published: April 2010

Abstract. In-situ observations of atmospheric CO2 and CH4 at Hateruma Island, Japan show large synoptic scale variations during a 6-month period from November to April, when the sampled air is predominantly of continental origin due to the Asian winter monsoon. Synoptic scale variations are extracted from the daily averaged values for the years between 1996 and 2007, along with the annual standard deviations (σCO2 and σCH4 for CO2 and CH4, respectively) for the relevant 6-month period. The temporal change in σCO2 shows a systematically increasing trend over the 12-year period, with elevated excursions in 1998 and 2003; there is no clear trend in σCH4. We also find that the σCO2/σCH4 ratio increases gradually from 1996 to 2002 and rapidly thereafter 2002 without any extreme deviations that characterized σCO2. The σCO2/σCH4 ratio correlates closely with the recent rapid increase in fossil carbon emission from China, as indicated in the CDIAC data. This methodology can be applied for tracking overall changes in regional emissions by measuring multiple chemical tracers.
Measuring condensation sink and ion sink of atmospheric aerosols with the electrical low pressure impactor (ELPI)
Authors: Kuuluvainen H. , Kannosto J. , Virtanen A. , Mäkelä J. M. , Kulmala M. , Aalto P. , Keskinen J.
Published: April 2010

Abstract. We investigate the suitability of ELPI for condensation sink and ion sink measurements. The aim is to find the simple calibration factors by which the measured ELPI currents can be converted to condensation or ion sinks. The calibration is based on DMPS and ELPI measurements within the period 15–25 May 2005 at a boreal forest site in Southern Finland. The values of condensation sink and ion sink were calculated from the DMPS size distributions using their theoretical definitions. After that the values were compared to theoretical and measured ELPI current, and calibration factors were specified. For condensation sink the calibration factor was found to be 7.27 E-06 s−1 fA−1 and for ion sink 7.33 E-06 s−1 fA−1. Simply by multiplying the total current of the outdoor ELPI by these factors, the values of condensation sink and ion sink can be measured.
Investigation of downscaling techniques for the linkage of global and regional air quality modeling
Authors: Lam Y. F. , Fu J. S.
Published: April 2010

Abstract. Recent year, downscaling global atmospheric model outputs for the USEPA Community Multiscale Air Quality (CMAQ) Initial (IC) and Boundary Conditions (BC) have become practical because of the rapid growth of computational technologies that allow global simulations can be completed within a reasonable time and have better performance. The traditional method of generating IC/BC by profile data has lost its advocators due to the weakness of the limited horizontal and vertical variations found on the gridded boundary layers. In this paper, we are in effort to investigate the effects of using profile IC/BC and global atmospheric model data. We utilize the GEOS-Chem model outputs to generate time-varied and layer-varied IC/BC for year 2002 using our newly development of tropopause determining algorithm. The purpose of the study is to determine the tropopause effect to the downscaling process. From the results, we have found that without considering tropopause in the downscaling process created unrealistic O3 concentrations in IC/BC at the upper boundary conditions for regional tropospheric model. This phenomenon has caused over-prediction of surface O3 in CMAQ. And it is greatly affected by temperature and latitudinal location. With the implementation of our algorithm, we have successfully resolved the incompatibility issues in the vertical layer structure between global and regions chemistry models to yield better surface O3 predictions than profile IC/BC on both summer and winter conditions. At the same time, it improved the vertical O3 distribution of CMAQ outputs. The algorithm can be applied to a global atmospheric model which performs a reasonable outcome to determine the tropopause.
Source classification of upper tropospheric pollution by MIPAS HCN and C2H6 global distributions
Authors: Glatthor N. , von Clarmann T. , Stiller G. P. , Funke B. , Koukouli M. E. , Fischer H. , Grabowski U. , Höpfner M. , Kellmann S. , Linden A.
Published: April 2010

Abstract. We present global upper tropospheric HCN and C2H6 amounts derived from MIPAS/ENVISAT limb emission spectra. HCN and C2H6 are retrieved in the spectral regions 715.5–782.7 cm−1 and 811.5–835.7 cm−1, respectively. The datasets we present consist of 54 days between September 2003 and March 2004. This period covers the peak and decline of the southern hemispheric biomass burning period and some months thereafter. HCN is a nearly unambiguous tracer of biomass burning with an assumed tropospheric lifetime of several months. Indeed, the most significant feature in the MIPAS HCN dataset is an upper tropospheric plume of enhanced values caused by southern hemispheric biomass burning, which in September and October 2003 extended from tropical South America over Africa, Australia to the Southern Pacific. The spatial extent of this plume agrees well with the MOPITT CO distribution of September 2003. Further there is good agreement with the shapes and mixing ratios of the southern hemispheric HCN and C2H6 fields measured by the ACE experiment between September and November 2005. The MIPAS HCN plume extended from the lowermost observation height (8 km) up to about 16 km altitude, with maximum values of 500–600 pptv in October 2003. It was still clearly visible in December 2003, but had strongly decreased by March 2004, confirming the assumed tropospheric lifetime. The main sources of C2H6 are production and transmission of fossil fuels, followed by biofuel use and biomass burning. The C2H6 distribution also clearly reflected the southern hemispheric biomass burning plume and its seasonal variation, with maximum amounts of 600–700 pptv. Generally there was good agreement between the southern hemispheric distributions of both pollution tracers, except for the region between Peru and the mid-Pacific. Here C2H6 was considerably enhanced, whereas the HCN amounts were low. Backward trajectory calculations suggested that industrial pollution was responsible for the elevated C2H6 in these particular air masses. Except for the Asian monsoon anticyclone in September 2003, there were only comparably small regions of enhanced HCN in the Northern Hemisphere. However, C2H6 showed an equally strong northern hemispheric signal between the equator and low midlatitudes, persisting over the whole observation period. Backward trajectory calculations for air masses from this region also pointed to industrial sources of this pollution. Generally, C2H6/HCN ratios between 1 and 1.5 indicate biomass burning and ratios larger than 1.5 industrial pollution. However, in March 2004 ratios of up to 2 were also found in some regions of the former southern biomass burning plume.
Towards closing the gap between hygroscopic growth and CCN activation for secondary organic aerosols – Part 3: Influence of the chemical composition on the hygroscopic properties and volatile fractions of aerosols
Authors: Poulain L. , Wu Z. , Petters M. D. , Wex H. , Hallbauer E. , Wehner B. , Massling A. , Kreidenweis S. M. , Stratmann F.
Published: April 2010

Abstract. The influence of varying levels of water mixing ratio, r, during the formation of secondary organic aerosol (SOA) from the ozonolysis of α-pinene on the SOA hygroscopicity and volatility was investigated. The reaction proceeded and aerosols were generated in a mixing chamber and the hygroscopic characteristics of the SOA were determined with LACIS (Leipzig Aerosol Cloud Interaction Simulator) and a Cloud Condensation Nuclei counter (CCNc). In parallel, a High-Resolution Time-of-Flight Aerodyne Aerosol Mass Spectrometer (HR-ToF-AMS) located downstream of a thermodenuder (TD) sampling from the mixing chamber, to collect mass spectra of particles from the volatile and non-volatile fractions of the SOA. Results showed that both hygroscopic growth and the volatile fraction of the SOA increased with increases in r inside the mixing chamber during SOA generation. An effective density of 1.40 g cm−3 was observed for the generated SOA when the reaction proceeded with r>1 g kg−1. Changes in the concentrations of the fragment CO2+ and the sum of CxHyOz+ (short name CHO) and CxHy+ (short name CH) fragments as measured by the HR-ToF-AMS were used to estimate changes in the oxidation level of the SOA with reaction conditions, using the ratios CO2+ to CH and CHO to CH. Under humid conditions, both ratios increased, corresponding to the presence of more oxygenated functional groups (i.e., carboxylic groups). This result is consistent with the α-pinene ozonolysis mechanisms which suggest that water interacts with the stabilized Criegee intermediate. The volatility and the hygroscopicity results show that SOA generation via ozonolysis of α-pinene in the presence of water vapour (r<16.884 g kg−1) leads to the formation of more highly oxygenated compounds that are more hygroscopic and more volatile than compounds formed under dry conditions.
Measurements of volatile organic compounds in the middle of Central East China during Mount Tai Experiment 2006 (MTX2006): observation of regional background and impact of biomass burning
Authors: Suthawaree J. , Kato S. , Okuzawa K. , Kanaya Y. , Pochanart P. , Akimoto H. , Wang Z. , Kajii Y.
Published: April 2010

Abstract. The measurement of volatile organic compounds (VOCs) was carried out at the summit of Mount Tai, located in the center of the Central East China (CEC) region, in June 2006 as part of the Mount Tai Experiment 2006 (MTX2006), which focused on the ozone and aerosol chemistry in the region. Temporal variations of simple VOCs between June 2 and June 28 revealed the characteristics of an aged air mass with minimum local influence. A comparison of VOCs observed at Mount Tai with other Chinese sites revealed relatively similar VOC levels to remote sites and, as expected, a lower level compared to more polluted sites. However, relatively high acetylene and benzene levels at Mount Tai were evidently indicated from comparison with normalized VOC profile by ethane suggested for Beijing. Owing to a shift in boundary layer height, we observed considerable differences between daytime and nighttime VOC concentrations. This suggests that the site has a very useful characteristic of being able to measure regional polluted air and the free troposphere regional background air quality. Influence of emissions from biomass burning in the region was evidently found to be extensive during the first half of the campaign (2–15 June), using fire spot data coupling with backward trajectory analysis. Agricultural residue burning was suggested as the primary source of emissions elucidated by the slope of the correlation plot between CH3Cl and CO obtained during the first half of the campaign.
Global model simulations of air pollution during the 2003 European heat wave
Authors: Ordóñez C. , Elguindi N. , Stein O. , Huijnen V. , Flemming J. , Inness A. , Flentje H. , Katragkou E. , Moinat P. , Peuch V.-H. , Segers A. , Thouret V. , Athier G. , van Weele M. , Zerefos C. S. , Cammas J.-P. , Schultz M. G.
Published: April 2010

Abstract. Three global Chemistry Transport Models – MOZART, MOCAGE, and TM5 – as well as MOZART coupled to the IFS meteorological model including assimilation of ozone (O3) and carbon monoxide (CO) satellite column retrievals, have been compared to surface measurements and MOZAIC vertical profiles in the troposphere over Europe for summer 2003. The models reproduce the meteorological features and enhancement of pollution in the troposphere over Central and Western Europe during the period 2–14 August, but not fully the ozone and CO mixing ratios measured during that episode. Modified normalised mean biases are around −25% (except ~5% for MOCAGE) in the case of ozone and from −80% to −30% in the case of CO in the boundary layer above Frankfurt. The coupling and assimilation of CO columns from MOPITT overcomes some of the deficiencies in the treatment of transport, chemistry and emissions in MOZART, reducing the negative biases to around 20%. Results from sensitivity simulations indicate that an increase of the coarse resolution of the global models to around 1°×1° and potential uncertainties in European anthropogenic emissions or in long-range transport of pollution cannot completely account for the underestimation of CO and O3 found for most global models. A process-oriented TM5 sensitivity simulation where soil wetness was reduced results in a decrease in dry deposition fluxes and a subsequent ozone increase larger than those of other sensitivity runs where the horizontal resolution or European emissions are increased. However this latest simulation still underestimates ozone during the heat wave and overestimates it outside that period. Most probably, a combination of the mentioned factors together with underrepresented biogenic emissions in the models, uncertainties in the modelling of vertical/horizontal transport processes in the proximity of the boundary layer as well as limitations of the chemistry schemes are responsible for the underestimation of ozone and CO found in most of the models during this extreme pollution event.
Organic nitrogen in PM2.5 aerosol at a forest site in the Southeast US
Authors: Lin M. , Walker J. , Geron C. , Khlystov A.
Published: April 2010

Abstract. There is growing evidence that organo-nitrogen compounds may constitute a significant fraction of the aerosol nitrogen (N) budget. However, very little is known about the abundance and origin of this aerosol fraction. In this study, the concentration of organic nitrogen (ON) and major inorganic ions in PM2.5 aerosol were measured at the Duke Forest Research Facility near Chapel Hill, NC, during January and June of 2007. A novel on-line instrument was used, which is based on the Steam Jet Aerosol Collector (SJAC) coupled to an on-line total carbon/total nitrogen analyzer and two on-line ion chromatographs. The concentration of ON was determined by tracking the difference in concentrations of total nitrogen and of inorganic nitrogen (determined as the sum of N-ammonium and N-nitrate). The time resolution of the instrument was 30 min with a detection limit for major aerosol components of ~0.1 μg m−3. Nitrogen in organic compounds contributed ~33% on average to the total nitrogen concentration in PM2.5, illustrating the importance of this aerosol component. Absolute concentrations of ON, however, were relatively low (<1.0 μg m−3) with an average of 0.18 μg m−3. The absolute and relative contribution of ON to the total aerosol nitrogen budget was practically the same in January and June. In January, the concentration of ON tended to be higher during the night and early morning, while in June it tended to be higher during the late afternoon and evening. Back-trajectories and correlation with wind direction indicate higher concentrations of ON in continental air than in marine air masses and indicate a variety of potential sources.
Closing the Dimethyl Sulfide Budget in the Tropical Marine Boundary Layer during the Pacific Atmospheric Sulfur Experiment
Authors: Conley S. A. , Faloona I. , Miller G. H. , Blomquist B. , Lenschow D. , Bandy A.
Published: April 2010

Abstract. Fourteen research flights were conducted with the National Center for Atmospheric Research (NCAR) C-130 near Christmas Island (2° N, 157° W) during the summer of 2007 as part of the Pacific Atmospheric Sulfur Experiment (PASE). In order to tightly constrain the scalar budget of DMS, fluxes were measured at various levels in the marine boundary layer (MBL) from near the surface (30 m) to the top of the mixed layer (500 m) providing greater accuracy of the flux divergence calculation in the DMS budget. The observed mean mole fraction of DMS in the MBL exhibited the well known diurnal cycle, ranging from 50 pptv in the daytime to 110 pptv at night. Contributions from horizontal advection are included using a multivariate regression of all DMS flight data from within the MBL to estimate the mean gradients and trends. With this technique we consider the residual term in the DMS budget as an estimate of overall photochemical oxidation. Error analysis of the various terms in the DMS budget indicate that chemical losses acting on time scales of up to 110 h can be inferred with this technique. On average, photochemistry accounted for 7.3 ppt hr−1 loss rate for the seven daytime flights, with an estimated error of 0.6 ppt/hr. The loss rate due to expected OH oxidation is sufficient to explain the net DMS destruction without invoking the action of additional oxidants (e.g. reactive halogens.) The observed ocean flux of DMS averaged 3.1 (±1.5)μmol m−2 d−1, and generally decreased throughout the sunlit hours. The average entrainment flux at the top of the MBL was 2.5 μmol m−2 d−1; therefore the flux divergence term in the budget equation only contributed an average increase of 1.3 ppt hr−1 to the mean MBL mole fraction. Over the entire mission, the horizontal advection contribution to the overall budget was 0.2 ppt hr−1, indicating a mean atmospheric DMS gradient nearly perpendicular to the east-southeasterly trade winds and the chlorophyll gradient in the equatorial upwelling ocean. Nonetheless, horizontal advection was a significant term in the budget of any given flight, ranging from −1.5 to 2.3 ppt hr−1, indicating a patchy and random seawater DMS distribution, and thus needs to be accounted for in budget studies.
Regional N2O fluxes in Amazonia derived from aircraft vertical profiles
Authors: D'Amelio M. T. S. , Gatti L. V. , Miller J. B. , Tans P.
Published: April 2010

Abstract. Nitrous oxide (N2O) is the third most important anthropogenic greenhouse gas. Globally, the main sources of N2O are nitrification and denitrification in soils. About two thirds of the soil emissions occur in the tropics and approximately 20% originate in wet rainforest ecosystems, like the Amazon forest. The work presented here involves aircraft vertical profiles of N2O from the surface to 4 km over two sites in the Eastern and Central Amazon: Tapajós National Forest (SAN) and Cuieiras Biologic Reserve (MAN), and the estimation of N2O fluxes for regions upwind of these sites. To our knowledge, these regional scale N2O measurements in Amazonia are unique and represent a new approach to looking regional scale emissions. The fluxes upwind of MAN exhibited little seasonality, and the annual mean was 2.1±1.0 mg N2O m−2 day−1, higher than that for fluxes upwind of SAN, which averaged 1.5±1.6 mg N2O m−2 day−1. The higher rainfall around the MAN site could explain the higher N2O emissions. For fluxes from the coast to SAN seasonality is present for all years, with high fluxes in the months of March through May, and in November through December. The first peak of N2O flux is strongly associated with the wet season. The second peak of high N2O flux recorded at SAN occurs during the dry season and can not be easily explained. However, about half of the dry season profiles exhibit significant correlations with CO, indicating a larger than expected source of N2O from biomass burning. The average CO:N2O ratio for all profiles sampled during the dry season is 94±77 mol CO:mol N2O and suggests a larger biomass burning contribution to the global N2O budget than previously reported.
The impact of aerosols on polarized sky radiance: model development, validation, and applications
Authors: Emde C. , Buras R. , Mayer B. , Blumthaler M.
Published: April 2010

Abstract. Although solar radiation initially is unpolarized when entering the Earth's atmosphere, it is polarized by scattering processes with molecules, water droplets, ice crystals, and aerosols. Hence, measurements of the polarization state of radiation can be used to improve remote sensing of aerosols and clouds. The analysis of polarized radiance measurements requires an accurate radiative transfer model. To this end, a new efficient and flexible three-dimensional Monte Carlo code to compute polarized radiances has been developed and implemented into MYSTIC (Monte Carlo code for the phYSically correct Tracing of photons In Cloudy atmospheres). Unlike discrete ordinate methods the Monte Carlo approach allows to handle the scattering phase matrices of aerosol and cloud particles accurately, i.e. without any approximations except the inherent statistical noise. The study presented in this paper shows that this is important, especially in order to simulate scattering by aerosols and cloud droplets in the ultraviolet wavelength region. The commonly used Delta-M approximation may cause large errors not only in the calculated intensity but also in the degree of polarization. The polarized downwelling radiation field is calculated for various aerosol types showing the high sensitivity of polarized ultraviolet radiances to the particle microphysics. Model simulations are compared to ground based measurements and found to be generally in good agreement. This comparison shows that there is a high potential to retrieve information about the aerosol type from polarized radiance measurements.
Characterization of a large biogenic secondary organic aerosol event from eastern Canadian forests
Authors: Slowik J. G. , Stroud C. , Bottenheim J. W. , Brickell P. C. , Chang R. Y.-W. , Liggio J. , Makar P. A. , Martin R. V. , Moran M. D. , Shantz N. C. , Sjostedt S. J. , van Donkelaar A. , Vlasenko A. , Wiebe H. A. , Xia A. G. , Zhang J. , Leaitch W. R. , Abbatt J. P. D.
Published: April 2010

Abstract. Biogenic secondary organic aerosol levels many times larger than past observations have been measured 70 km north of Toronto during a period of increasing temperatures and outflow from Northern Ontario and Quebec forests in early summer. A regional chemical transport model approximately predicts the event timing and accurately predicts the aerosol loading, identifying the precursors as monoterpene emissions from the coniferous forest. The agreement between the measured and modeled biogenic aerosol concentrations contrasts with model underpredictions for polluted regions. Correlations of the oxygenated organic aerosol mass with tracers such as CO support a secondary aerosol source and distinguish biogenic, pollution, and biomass burning periods during the field campaign. Using the Master Chemical Mechanism, it is shown that the levels of CO observed during the biogenic event are consistent with a photochemical source arising from monoterpene oxidation. The biogenic aerosol mass correlates with satellite measurements of regional aerosol optical depth, indicating that the event extends across the eastern Canadian forest. This regional event correlates with increased temperatures, indicating that temperature-dependent forest emissions can significantly affect climate through enhanced direct radiative forcing and higher cloud condensation nuclei numbers.
Wildfire smoke in the Siberian Arctic in summer: source characterization and plume evolution from airborne measurements
Authors: Paris J.-D. , Stohl A. , Nédélec P. , Arshinov M. Yu. , Panchenko M. V. , Shmargunov V. P. , Law K. S. , Belan B. D. , Ciais P.
Published: April 2010

Abstract. We present airborne measurements of carbon dioxide (CO2), carbon monoxide (CO), ozone (O3), equivalent black carbon (EBC) and ultra fine particles over North-Eastern Siberia in July 2008 performed during the YAK-AEROSIB/POLARCAT experiment. During a "golden day" (11 July 2008) a number of biomass burning plumes were encountered with CO concentration enhancements of up to 500 ppb relative to a background of 90 ppb. Number concentrations of aerosols in the size range 3.5–200 nm peaked at 4000 cm−3 and the EBC content reached 1.4 μg m−3. These high concentrations were caused by forest fires in the vicinity of the landing airport in Yakutsk where during the descent measurements in fresh smoke could be made. We estimate a combustion efficiency of 90±3% based on CO and CO2 measurements. The emission factor of CO emitted was 59.6±15.2 g CO per kilogram of dry matter burned, suggesting an increase in the average northern hemispheric CO concentration of 3.0–7.2 ppb per million hectares of Siberian forest burned. For BC, we estimate an emission factor of 0.52±0.07 g BC kg−1, comparable to values reported in the literature. The emission ratio of ultra-fine particles (3.5–200 nm) was 26 cm−3 (ppb CO)−1, consistent with other airborne studies. The transport of identified biomass burning plumes was investigated using the FLEXPART Lagrangian model. Based on sampling of wildfire plumes from the same source but with different atmospheric ages derived from FLEXPART, we estimate that the e-folding lifetimes of EBC and ultra fine particles (between 3.5 and 200 nm in size) against removal and growth processes are 5.1 and 5.5 days, respectively, supporting lifetimes estimates used in various modelling studies.
Results from the CERN pilot CLOUD experiment
Authors: Duplissy J. , Enghoff M. B. , Aplin K. L. , Arnold F. , Aufmhoff H. , Avngaard M. , Baltensperger U. , Bondo T. , Bingham R. , Carslaw K. , Curtius J. , David A. , Fastrup B. , Gagné S. , Hahn F. , Harrison R. G. , Kellett B. , Kirkby J. , Kulmala M. , Laakso L. , Laaksonen A. , Lillestol E. , Lockwood M. , Mäkelä J. , Makhmutov V. , Marsh N. D. , Nieminen T. , Onnela A. , Pedersen E. , Pedersen J. O. P. , Polny J. , Reichl U. , Seinfeld J. H. , Sipilä M. , Stozhkov Y. , Stratmann F. , Svensmark H. , Svensmark J. , Veenhof R. , Viisanen Y. , Wagner P. E. , Wehrle G. , Weingartner E. , Wex H. , Wilhelmsson M. , Winkler P. M.
Published: April 2010

Abstract. During a 4-week run in October–November 2006, a pilot experiment was performed at the CERN Proton Synchrotron in preparation for the CLOUD1 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 H2SO4 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). 1CLOUD is an acronym of Cosmics Leaving OUtdoor Droplets.
Observations of high rates of NO2 – HONO conversion in the nocturnal atmospheric boundary layer in Kathmandu, Nepal
Authors: Yu Y. , Galle B. , Hodson E. , Panday A. , Prinn R. , Wang S.
Published: April 2010

Abstract. Nitrous acid (HONO) plays a significant role in the atmosphere, especially in the polluted troposphere. Its photolysis after sunrise is an important source of hydroxyl free radicals (OH). Measurements of nitrous acid and other pollutants were carried out in the Kathmandu urban atmosphere during January–February 2003, contributing to the sparse knowledge of nitrous acid in South Asia. The results showed average nocturnal levels of HONO (1.7±0.8 ppbv), NO2 (17.9±10.2 ppbv), and PM10 (0.18±0.11 mg m−3) in urban air in Kathmandu. Surprisingly high ratios of chemically formed secondary [HONO] to [NO2] (up to 30%) were found, which indicates unexpectedly efficient chemical conversion of NO2 to HONO in Kathmandu. The ratios of [HONO]/[NO2] at nights are much higher than previously reported values from measurements in urban air in Europe, North America and Asia. The influence of aerosol plumes, relative humidity, aerosol surface and ground reactive surface, temperature on NO2-HONO chemical conversion were discussed. The high humidity, strong and low inversion layer at night, and serious aerosol pollution burden may explain the particularly efficient conversion of NO2 to HONO.
Transport and vertical structure of aerosols and water vapor over West Africa during the African monsoon dry season
Authors: Kim S.-W. , Chazette P. , Dulac F. , Sanak J. , Johnson B. , Yoon S.-C.
Published: April 2010

Abstract. We present observations of tropospheric aerosol and water vapor transport over West Africa and the associated meteorological conditions during the AMMA SOP-0 dry season experiment, which was conducted in West Africa in January–February 2006. This study combines data from ultra-light aircraft (ULA)-based lidar, airborne in-situ aerosol and gas measurements, standard meteorological measurements, satellite-based aerosol measurements, airmass trajectories, and radiosonde measurements. At Niamey (13.5° N, 2.2° E) the prevailing surface wind was from the northeast bringing dry dusty air from the Sahara desert. High concentrations of mineral dust aerosol were typically observed from the surface to 1.5 or 2 km associated with the Saharan airmasses. At higher altitudes the prevailing wind veered to the south or southeast bringing relatively warm and humid airmasses from the biomass burning regions to the Sahel (<10° N). These elevated layers had high concentrations of biomass burning aerosol and were typically observed between altitudes of 2–5 km. Meteorological analyses show these airmasses were advected upwards over the biomass burning regions through large-scale ascent, presumably driven by surface heating rather than pyro-convection. Aerosol vertical profiles obtained from the space-based lidar CALIOP onboard CALIPSO during January 2007 also showed the presence of dust particles (depolarization ~30%, color ratio <0) at low levels (<1.5 km) and biomass burning smoke aerosol (depolarization ratio <10%) between 2 and 5 km. CALIOP data indicated that these distinct continental dust and biomass burning aerosol layers likely mixed as they advected further south over the tropical Atlantic Ocean.
Technical Note: Scintillations of the double star α Cru observed by GOMOS/Envisat
Authors: Sofieva V. F. , Dalaudier F. , Kan V. , Gurvich A. S.
Published: April 2010

Abstract. In this paper, we discuss scintillation time-spectra of the double star α Cru, which were measured by the GOMOS/Envisat photometer. The components of α Cru are not resolved by the angular field of view of the detector. The double structure of the light source reveals itself in the modulation of the observed scintillation spectra; this modulation is caused by anisotropic irregularities of stratospheric air density. We present qualitative and quantitative explanation of properties of the double-star scintillation spectra. Possibilities of using double star scintillations for studying atmospheric air density irregularities are also discussed in the paper.
Lagrangian mixing in an axisymmetric hurricane model
Authors: Rutherford B. , Dangelmayr G. , Persing J. , Kirby M. , Montgomery M.T.
Published: April 2010

Abstract. This paper discusses the extension of established Lagrangian mixing measures to make them applicable to data extracted from a 2-D axisymmetric hurricane simulation. Because of the non-steady and unbounded characteristics of the simulation, the previous measures are extended to a moving frame approach to create time-dependent mixing rates that are dependent upon the initial time of particle integration, and are computed for nonlocal regions. The global measures of mixing derived from finite-time Lyapunov exponents, relative dispersion, and a measured mixing rate are applied to distinct regions representing different characteristic feautures within the model. It is shown that these time-dependent mixing rates exhibit correlations with maximal tangential winds during a quasi-steady state, establishing a connection between mixing and hurricane intensity.
Metal concentrations in the upper atmosphere during meteor showers
Authors: Correira J. , Aikin A. C. , Grebowsky J. M. , Burrows J. P.
Published: April 2010

Abstract. Using the nadir-viewing Global Ozone Measuring Experiment (GOME) UV/VIS spectrometer on the ERS-2 satellite, we investigate short term variations in the vertical magnesium column densities in the atmosphere and any connection to possible enhanced mass deposition during a meteor shower. Time-dependent mass influx rates are derived for all the major meteor showers using published estimates of mass density and temporal profiles of meteor showers. An average daily sporadic background mass flux rate is also calculated and used as a baseline against which calculated shower mass flux rates are compared. These theoretical mass flux rates are then compared with GOME derived metal vertical column densities of Mg and Mg+ from the years 1996–2001. There is no correlation between theoretical mass flux rates and changes in the Mg and Mg+ metal column densities. A possible explanation for the lack of a shower related increase in metal concentrations may be differences in the mass regimes dominating the average background mass flux and shower mass flux.
Peroxy radicals and ozone photochemistry in air masses undergoing long-range transport
Authors: Parker A. E. , Monks P. S. , Jacob M. J. , Penkett S. A. , Lewis A. C. , Stewart D. J. , Whalley L. K. , Methven J. , Stohl A.
Published: April 2010

Abstract. Concentrations of peroxy radicals (HO2+ΣiRiO2) in addition to other trace gases were measured onboard the UK Meteorological Office/Natural Environment Research Council British Aerospace 146-300 atmospheric research aircraft during the Intercontinental Transport of Ozone and Precursors (ITOP) campaign based at Horta Airport, Faial, Azores (38.58° N, 28.72° W) in July/August 2004. The overall peroxy radical altitude profile displays an increase with altitude that is likely to have been impacted by the effects of long-range transport. The peroxy radical altitude profile for air classified as of marine origin shows no discernable altitude profile. A range of air-masses were intercepted with varying source signatures, including those with aged American and Asian signatures, air-masses of biomass burning origin, and those that originated from the east coast of the United States. Enhanced peroxy radical concentrations have been observed within this range of air-masses indicating that long-range transported air-masses traversing the Atlantic show significant photochemical activity. The net ozone production at clear sky limit is in general negative, and as such the summer mid-Atlantic troposphere is at limit net ozone destructive. However, there is clear evidence of positive ozone production even at clear sky limit within air masses undergoing long-range transport, and during ITOP especially between 5 and 5.5 km, which in the main corresponds to a flight that extensively sampled air with a biomass burning signature. Ozone production was NOx limited throughout ITOP, as evidenced by a good correlation (r2=0.72) between P(O3) and NO. Strong positive net ozone production has also been seen in varying source signature air-masses undergoing long-range transport, including but not limited to low-level export events, and export from the east coast of the United States.
Methane and nitrous oxide emissions in The Netherlands: ambient measurements support the national inventories
Authors: van der Laan S. , Neubert R. E. M. , Meijer H. A. J.
Published: April 2010

Abstract. We present net emission estimates of CH4 and N2O of The Netherlands based on measurements conducted during the period of May 2006 to April 2009 at station Lutjewad, The Netherlands (6° 21' E, 53° 24' N, 1 m a.s.l.). 222Radon mixing ratios were applied as an indicator for vertical mixing and long-range air mass transport and used to calculate the net surface fluxes from atmospheric mixing ratios of CH4 and N2O. Our study shows that our measurement site Lutjewad is well-suited to measure emissions from The Netherlands and validation of the national inventories using the 222Radon flux method. Since this study is purely observation-based it is independent from inventories or atmospheric models. Our results are compared to the national inventories as reported to the UNFCCC. We found net emissions of: (15.2±5.3) t km-2 a-1 for CH4 and (0.9±0.3) t km-2 a-1 for N2O. These values are lower than the inventory-based emissions (2006–2008 averages) of (18.3±3.3) t km-2 a-1 for CH4, and (1.3±0.6) t km-2 a-1 for N2O, but the differences are insignificant.
Oxidant and particle photochemical processes above a south-east Asian tropical rain forest (the OP3 project): introduction, rationale, location characteristics and tools
Authors: Hewitt C. N. , Lee J. , Barkley M. P. , Carslaw N. , Chappell N. A. , Coe H. , Collier C. , Commane R. , Davies F. , DiCarlo P. , Di Marco C. F. , Edwards P. M. , Evans M. J. , Fowler D. , Furneaux K. L. , Gallagher M. , Guenther A. , Heard D. E. , Helfter C. , Hopkins J. , Ingham T. , Irwin M. , Jones C. , Karunaharan A. , Langford B. , Lewis A. C. , Lim S. F. , MacDonald S. M. , MacKenzie A. R. , Mahajan A. S. , Malpass S. , McFiggans G. , Mills G. , Misztal P. , Moller S. , Monks P. S. , Nemitz E. , Nicolas-Perea V. , Oetjen H. , Oram D. , Palmer P. I. , Phillips G. J. , Plane J. M. C. , Pugh T. , Pyle J. A. , Reeves C. E. , Robinson N. H. , Stewart D. , Stone D. , Whalley L. K.
Published: April 2010

Abstract. In April–July 2008, intensive measurements were made of atmospheric composition and chemistry in Sabah, Malaysia, as part of the "Oxidant and particle photochemical processes above a South-East Asian tropical rain forest" (OP3) project. Fluxes and concentrations of trace gases and particles were made from and above the rain forest canopy at the Bukit Atur Global Atmosphere Watch station and at the nearby Sabahmas oil palm plantation, using both ground-based and airborne measurements. Here, the measurement and modelling strategies used, the characteristics of the sites and an overview of data obtained are described. Composition measurements show that the rainforest site was not impacted by significant sources of anthropogenic pollution, and this is confirmed by satellite retrievals of NO2 and HCHO. The dominant modulators of atmospheric chemistry at the rain forest site were therefore emissions of BVOCs and soil emissions of reactive nitrogen oxides. At the observed BVOC:NOx volume mixing ratio (~104 pptv/pptv), current chemical models suggest that daytime maximum OH concentrations should be ca. 105 radicals cm−3, but observed OH concentrations were an order of magnitude greater than this. We confirm, therefore, previous measurements which suggest that an unexplained source of OH must exist above tropical forests and continue to interrogate the data to find explanations for this.
Impacts of electronically photo-excited NO2 on air pollution control strategies in the South Coast Air Basin of California
Authors: Ensberg J. J. , Carreras-Sospedra M. , Dabdub D.
Published: April 2010

Abstract. A new path for hydroxyl radical formation via photo-excitation of nitrogen dioxide (NO2) and the reaction of photo-excited NO2 with water is evaluated using the UCI-CIT model for the South Coast Air Basin of California (SoCAB). Two separate studies predict different reaction rates, which differ by nearly an order of magnitude, for the reaction of photo-excited NO2 with water. Impacts of this new chemical mechanism on ozone and particulate matter formation, while utilizing both reaction rates, are quantified by simulating a two-day summer episode. In addition, sensitivity simulations are conducted to evaluate the uncertainty in the rate of reaction of photo-excited NO2 with water reported in the literature. Results indicate that the addition of photo-excited NO2 chemistry increases peak 1-h average ozone concentrations by up to 20.6%. Also, the new chemistry leads to moderate increases in particulate matter concentrations of up to 2.9%. The importance of this new chemistry is then evaluated in the context of pollution control strategies. A series of simulations are conducted to generate isopleths for ozone and particulate matter concentrations, varying baseline nitrogen oxides (NOx) and volatile organic compounds emissions. Results show that including NO2 photo-excitation increases the sensitivity of ozone concentration to changes in NOx emissions. Namely, increasing NOx when NO2 photo-excitation is included, while utilizing the higher reaction rate, leads to an increase in ozone concentration of up to 38.7% higher than a case without photo-excited NO2. Ozone and particulate matter control strategies rely heavily on the variation of NOx and VOC emissions and the addition of the new chemical mechanism increases peak ozone and 24-h average PM concentrations in all locations under all NOx and VOC scaling factors while utilizing both reaction rates. Therefore, three-dimensional air quality models should be modified to include this new OH production mechanism, especially if used to develop emission controls strategies.
Objective assessment of ozone in chemistry-climate model simulations
Authors: Karpechko A. Yu. , Gillett N. P. , Hassler B. , Rosenlof K. H. , Rozanov E.
Published: April 2010

Abstract. Stratospheric ozone recovery is expected to drive pronounced trends in atmospheric temperature and circulation from the stratosphere to the troposphere in the 21st century, but coupled chemistry-climate models (CCMs) vary widely in their predictions of future ozone evolution. In order to assess which models might be expected to better simulate future ozone evaluation, we assess the ability of twelve CCMs to simulate observed ozone climatology and trends and rank the models according to their errors averaged across the individual diagnostics chosen. According to our analysis no one model performs better than the others in all the diagnostics; however, combining errors in individual diagnostics into one metric of model performance allows us to objectively rank the models. The multi-model average shows better overall agreement with the observations than any individual model. Based on this analysis we conclude that the multi-model average ozone projection presents the best estimate of future ozone evolution. Our results also demonstrate a sensitivity of the analysis to the choice of reference data set for vertical ozone distribution over the Antarctic, highlighting the constraints that large observational uncertainty imposes on such model verification.
Modeling of Saharan dust outbreaks over the Mediterranean by RegCM3: case studies
Authors: Santese M. , Perrone M. R. , Zakey A. S. , De Tomasi F. , Giorgi F.
Published: April 2010

Abstract. The regional climate model RegCM3 coupled with a radiatively active aerosol model with online feedback is used to investigate direct and semi-direct radiative aerosol effects over the Sahara and Europe in a test case of July 2003. The aerosol model includes dust particles in addition to sulfates, hydrophobic and hydrophilic black carbon and organic carbon. The role of the aerosol online feedback on the radiation budget and the direct radiative forcing (short-wave and long-wave) by dust particles are investigated by intercomparing results from three experiments: REF, including all interactive aerosol components, Exp1, not accounting for the aerosol radiative feedback, and Exp2 not accounting for desert dust particles. The comparison of results in the REF experiment with satellite observations, sun/sky radiometer measurements, and lidar profiles at selected Central Mediterranean sites reveals that the spatio-temporal evolution of the aerosol optical depth is reasonably well reproduced by the model during the entire month of July. Results for the dust outbreaks of 17 and 24 July, averaged over the simulation domain, show that the daily-mean SW direct radiative forcing by all particles is −24 W/m2 and −3.4 W/m2 on 17 July and −25 W/m2 and −3.5 W/m2 on 24 July at the surface and top of the atmosphere, respectively. This is partially offset by a LW direct radiative forcing of ~30% at the surface and of ~50% at the ToA. It is also shown that atmospheric dynamics and hence dust production and advection processes are dependent on the simulation assumptions and may significantly change within few tens of kilometers. The comparison of REF and Exp1 shows that the aerosol online feedback on the radiation budget decreases the domain-average daily-mean value of the 2 m-temperature, aerosol column burden (CB), and short-wave (SW) atmospheric forcing by 0.52°C, 14%, and 0.9%, respectively on 17 July and by 0.39°C, 12% and 12%, respectively on 24 July. The comparison of REF and Exp2 reveals that on 17 July, radiatively-active dust particles decrease the daily-mean 2-m temperature averaged over the whole simulation domain by 0.12°C even if are responsible for 99.8% and 97% of the daily-mean aerosol column burden and SW atmospheric forcing, respectively.
Estimates of biomass burning emissions in tropical Asia based on satellite-derived data
Authors: Chang D. , Song Y.
Published: April 2010

Abstract. Biomass burning in tropical Asia emits large amounts of trace gases and particulate matters into the atmosphere, which has significant implications for atmospheric chemistry and climatic change. In this study, emissions from open biomass burning over tropical Asia were evaluated during seven fire years from 2000–2006 (1 April 2000–31 March 2007). Burned areas were estimated from newly published 1-km L3JRC and 500-m MODIS burned area products (MCD45A1). Available fuel loads and emission factors were assigned for each vegetation type in a GlobCover characterisation map, and fuel moisture content was taken into account when calculating combustion factors. Over the whole period, both burned areas and fire emissions clearly showed spatial and seasonal variations. The L3JRC burned areas ranged from 31 165 km2 in fire year 2005 to 57 313 km2 in 2000, while the MCD45A1 burned areas ranged from 54 260 km2 in fire year 2001 to 127 068 km2 in 2004. Comparisons of L3JRC and MCD45A1 burned areas with ground-based measurements and other satellite information were constructed in several major burning regions, and results suggested that MCD45A1 performed better in most areas than L3JRC did although with a certain degree of underestimation of burned forest areas. The average annual L3JRC-based emissions were 125, 12, 0.98, 1.91, 0.11, 0.89, 0.044, 0.022, 0.42, 3.40, and 3.68 Tg yr