bluuebunny/crossref_metadata_2025 huggingface dataset:
CUACE/Dust – an integrated system of observation and modeling systems for operational dust forecasting in Asia
Authors: Gong S. L. , Zhang X. Y.
Published: April 2010

Abstract. An integrated sand and dust storm (SDS) forecasting system – CUACE/Dust (Chinese Unified Atmospheric Chemistry Environment for Dust) has been developed, which consists of a comprehensive dust aerosol module with emission, dry/wet depositions and other atmospheric dynamic processes, and a data assimilation system (DAS) using observational data from the CMA (China Meteorological Administration) ground dust monitoring network and retrieved dust information from a Chinese geostationary satellite – FY-2C. This is the first time that a combination of surface network observations and satellite retrievals of the dust aerosol has been successfully used in the real time operational forecasts in East Asia through a DAS. During its application for the operational SDS forecasts in East Asia for spring 2006, this system captured the major 31 SDS episodes observed by both surface and satellite observations. Analysis shows that the seasonal mean threat score (TS) for 0–24 h forecast over the East Asia in spring 2006 increased from 0.22 to 0.31 by using the DAS, a 41% enhancement. The time series of the forecasted dust concentrations for a number of representative stations for the whole spring 2006 were also evaluated against the surface PM10 monitoring data, showing a very good agreement in terms of the SDS timing and magnitudes near source regions where dust aerosols dominate. This is a summary paper for a special issue of ACP featuring the development and results of the forecasting system.
Ozone-enhanced layers in the troposphere over the equatorial Pacific Ocean and the influence of transport of midlatitude UT/LS air
Authors: Hayashi H. , Kita K. , Taguchi S.
Published: April 2010

Abstract. Occurrence of ozone (O3)-enhanced layers in the troposphere over the equatorial Pacific Ocean and their seasonal variation were investigated based on ozonesonde data obtained at three Southern Hemisphere ADditional OZonesondes (SHADOZ) sites, Watukosek, American Samoa and San Cristobal, for 6 years between 1998 and 2003. O3-enhanced layers were found in about 50% of observed O3 profiles at the three sites. The formation processes of O3-enhanced layers were investigated by meteorological analyses including backward trajectories. On numerous occasions, O3-enhanced layers resulted from the transport of air masses affected by biomass burning. The contribution of this process was about 30% at San Cristobal during the periods from February to March and from August to September, while it was relatively low, about 10%, at Watukosek and Samoa. A significant number of the O3-enhanced layers were attributed to the transport of midlatitude upper-troposphere and lower-stratosphere (UT/LS) air. Meteorological analyses indicated that these layers originated from equatorward and downward transport of the midlatitude UT/LS air masses through a narrow region between high- and low-pressure systems around the subtropical jet stream. This process accounted for 50–80% at Watukosek between May and December, about 80% at Samoa on yearly average, and 40–70% at San Cristobal between November and March, indicating that it was important for O3 budget over the equatorial Pacific Ocean.
Evaluation of the atmospheric transport in a GCM using radon measurements: sensitivity to cumulus convection parameterization
Authors: Zhang K. , Wan H. , Zhang M. , Wang B.
Published: April 2010

Abstract. The radioactive species radon (222Rn) has long been used as a test tracer for the numerical simulation of large scale transport processes. In this study, radon transport experiments are carried out using an atmospheric GCM with a finite-difference dynamical core, the van Leer type FFSL advection algorithm, and two state-of-the-art cumulus convection parameterization schemes. Measurements of surface concentration and vertical distribution of radon collected from the literature are used as references in model evaluation. The simulated radon concentrations using both convection schemes turn out to be consistent with earlier studies with many other models. Comparison with measurements indicates that at the locations where significant seasonal variations are observed in reality, the model can reproduce both the monthly mean surface radon concentration and the annual cycle quite well. At those sites where the seasonal variation is not large, the model is able to give a correct magnitude of the annual mean. In East Asia, where radon simulations are rarely reported in the literature, detailed analysis shows that our results compare reasonably well with the observations. The most evident changes caused by the use of a different convection scheme are found in the vertical distribution of the tracer. The scheme associated with weaker upward transport gives higher radon concentration up to about 6 km above the surface, and lower values in higher altitudes. In the lower part of the atmosphere results from this scheme does not agree as well with the measurements as the other scheme. Differences from 6 km to the model top are even larger, although we are not yet able to tell which simulation is better due to the lack of observations at such high altitudes.
Observations of shallow convective clouds generated by solar heating of dark smoke plumes
Authors: Klüser L. , Rosenfeld D. , Macke A. , Holzer-Popp T.
Published: April 2010

Abstract. The SEVIRI instrument on the Meteosat Second Generation satellite with both fine spatial and temporal resolution allows to detect and follow the dynamics of fast developing meteorological events like spreading smoke plumes and the lifecycles of convective clouds. Smoke plumes have the ability to change the atmospheric heat content due to absorption and reduced reflection of solar radiation. By these means they can trigger formation of shallow convective clouds at their edge. A heavy smoke plume emerging from burning Lebanese oil tanks and spreading over adjacent deserts on 17 July 2006 has been observed as an example of such an effect. This study suggests a physical explanation of the observed convection along the edge of the smoke plume, namely the strong thermal contrast resulting from solar heating of the smoke layer.
Adjoint inversion modeling of Asian dust emission using lidar observations
Authors: Yumimoto K. , Uno I. , Sugimoto N. , Shimizu A. , Liu Z. , Winker D. M.
Published: April 2010

Abstract. A four-dimensional variational (4D-Var) data assimilation system for a regional dust model (RAMS/CFORS-4DVAR; RC4) is applied to an adjoint inversion of a heavy dust event over eastern Asia during 20 March–4 April 2007. The vertical profiles of the dust extinction coefficients derived from NIES Lidar network are directly assimilated, with validation using observation data. Two experiments assess impacts of observation site selection: Experiment A uses five Japanese observation sites located downwind of dust source regions; Experiment B uses these and two other sites near source regions. Assimilation improves the modeled dust extinction coefficients. Experiment A and Experiment B assimilation results are mutually consistent, indicating that observations of Experiment A distributed over Japan can provide comprehensive information related to dust emission inversion. Time series data of dust AOT calculated using modeled and Lidar dust extinction coefficients improve the model results. At Seoul, Matsue, and Toyama, assimilation reduces the root mean square differences of dust AOT by 35–40%. However, at Beijing and Tsukuba, the RMS differences degrade because of fewer observations during the heavy dust event. Vertical profiles of the dust layer observed by CALIPSO are compared with assimilation results. The dense dust layer was trapped at potential temperatures (θ) of 280–300 K and was higher toward the north; the model reproduces those characteristics well. Latitudinal distributions of modeled dust AOT along the CALIPSO orbit paths agree well with those of CALIPSO dust AOT, OMI AI, and MODIS coarse-mode AOT, capturing the latitude at which AOTs and AI have high values. Assimilation results show increased dust emissions over the Gobi Desert and Mongolia; especially for 29–30 March, emission flux is about 10 times greater. Strong dust uplift fluxes over the Gobi Desert and Mongolia cause the heavy dust event. Total optimized dust emissions are 57.9 Tg (Experiment A; 57.8% larger than before assimilation) and 56.3 Tg (Experiment B; 53.4% larger).
Online-coupled meteorology and chemistry models: history, current status, and outlook
Authors: Zhang Y.
Published: April 2010

Abstract. The climate-chemistry-aerosol-cloud-radiation feedbacks are important processes occurring in the atmosphere. Accurately simulating those feedbacks requires fully-coupled meteorology, climate, and chemistry models and presents significant challenges in terms of both scientific understanding and computational demand. This paper reviews the history and current status of the development and application of online-coupled meteorology and chemistry models, with a focus on five representative models developed in the US including GATOR-GCMOM, WRF/Chem, CAM3, MIRAGE, and Caltech unified GCM. These models represent the current status and/or the state-of-the science treatments of online-coupled models worldwide. Their major model features, typical applications, and physical/chemical treatments are compared with a focus on model treatments of aerosol and cloud microphysics and aerosol-cloud interactions. Aerosol feedbacks to planetary boundary layer meteorology and aerosol indirect effects are illustrated with case studies for some of these models. Future research needs for model development, improvement, application, as well as major challenges for online-coupled models are discussed.
Analysis of aircraft and satellite measurements from the Intercontinental Chemical Transport Experiment (INTEX-B) to quantify long-range transport of East Asian sulfur to Canada
Authors: van Donkelaar A. , Martin R. V. , Leaitch W. R. , Macdonald A. M. , Walker T. W. , Streets D. G. , Zhang Q. , Dunlea E. J. , Jimenez J. L. , Dibb J. E. , Huey L. G. , Weber R. , Andreae M. O.
Published: April 2010

Abstract. We interpret a suite of satellite, aircraft, and ground-based measurements over the North Pacific Ocean and western North America during April–May 2006 as part of the Intercontinental Chemical Transport Experiment Phase B (INTEX-B) campaign to understand the implications of long-range transport of East Asian emissions to North America. The Canadian component of INTEX-B included 33 vertical profiles from a Cessna 207 aircraft equipped with an aerosol mass spectrometer. Long-range transport of organic aerosols was insignificant, contrary to expectations. Measured sulfate plumes in the free troposphere over British Columbia exceeded 2 μg/m3. We update the global anthropogenic emission inventory in a chemical transport model (GEOS-Chem) and use it to interpret the observations. Aerosol Optical Depth (AOD) retrieved from two satellite instruments (MISR and MODIS) for 2000–2006 are analyzed with GEOS-Chem to estimate an annual growth in Chinese sulfur emissions of 6.2% and 9.6%, respectively. Analysis of aircraft sulfate measurements from the NASA DC-8 over the central Pacific, the NSF C-130 over the east Pacific and the Cessna over British Columbia indicates most Asian sulfate over the ocean is in the lower free troposphere (800–600 hPa), with a decrease in pressure toward land due to orographic effects. We calculate that 56% of the measured sulfate between 500–900 hPa over British Columbia is due to East Asian sources. We find evidence of a 72–85% increase in the relative contribution of East Asian sulfate to the total burden in spring off the northwest coast of the United States since 1985. Campaign-average simulations indicate anthropogenic East Asian sulfur emissions increase mean springtime sulfate in Western Canada at the surface by 0.31 μg/m3 (~30%) and account for 50% of the overall regional sulfate burden between 1 and 5 km. Mean measured daily surface sulfate concentrations taken in the Vancouver area increase by 0.32 μg/m3 per 10% increase in the simulated fraction of Asian sulfate, and suggest current East Asian emissions episodically degrade local air quality by more than 1.5 μg/m3.
UV variability in Moscow according to long-term UV measurements and reconstruction model
Authors: Chubarova N. Y.
Published: April 2010

Abstract. Long-term measurements of erythemally weighted UV irradiance (Qer) have been analyzed for the 1999–2006 period as well as UV variability according to a reconstruction model since 1968. The estimates of different atmospheric parameters effects, including NO2 content, on Qer have been obtained on seasonal and interannual scales. It has been shown that NO2 content in conditions of large megalopolis provides average Qer decrease of about 1.5–2%. The seasonal variations of the observed UV indices are discussed from the point of view of the impact on health. Using the reconstruction model we showed a distinct growth in Qer since 1980 due to changes in total ozone (+2.5% per decade), effective cloud amount transmission (+2.1% per decade) and aerosol loading (+1.1% per decade). However, there is no change in Qer over the longer 1968–2006 period due to significant decrease in effective cloud amount transmission (−11% per decade) in 1968–1980.
Validation of stratospheric water vapour measurements from the airborne microwave radiometer AMSOS
Authors: Müller S. C. , Kämpfer N. , Feist D. G. , Haefele A. , Milz M. , Sitnikov N. , Schiller C. , Kiemle C. , Urban J.
Published: April 2010

Abstract. We present the validation of a water vapour dataset obtained by the Airborne Microwave Stratospheric Observing System AMSOS, a passive microwave radiometer operating at 183 GHz. Vertical profiles are retrieved from spectra by an optimal estimation method. The useful vertical range lies in the upper troposphere up to the mesosphere with an altitude resolution of 8 to 16 km and a horizontal resolution of about 57 km. Flight campaigns were performed once a year from 1998 to 2006 measuring the latitudinal distribution of water vapour from the tropics to the polar regions. The obtained profiles show clearly the main features of stratospheric water vapour in all latitudinal regions. Data are validated against a set of instruments comprising satellite, ground-based, airborne remote sensing and in-situ instruments. It appears that AMSOS profiles have a dry bias of 0 to –20%, when compared to satellite experiments. Also a comparison between AMSOS and in-situ hygrosondes FISH and FLASH have been performed. A matching in the short overlap region in the upper troposphere of the lidar measurements from the DIAL instrument and the AMSOS dataset allowed water vapour profiling from the middle troposphere up to the mesosphere.
Comparison of total ozone and erythemal UV data from OMI with ground-based measurements at Rome station
Authors: Ialongo I. , Casale G. R. , Siani A. M.
Published: April 2010

Abstract. Ground-based total ozone and surface UV irradiance measurements have been collected since 1992 using Brewer spectrophotometer at Rome station. Erythemal Dose Rates (EDRs) have been also determined by a broad-band radiometer (model YES UVB-1) operational since 2000. The methodology to retrieve the EDR and the Erythemal Daily Dose (EDD) from the radiometer observations is described. Ground-based measurements were compared with satellite-derived total ozone and UV data from the Ozone Monitoring Instrument (OMI). OMI, onboard the NASA EOS Aura spacecraft, is a nadir viewing spectrometer that provides total ozone and surface UV retrievals. The results of the validation exercise showed satisfactory agreement between OMI and Brewer total ozone data, for both OMI-TOMS and OMI-DOAS ozone algorithms (biases of −1.8% and −0.7%, respectively). Regarding UV data, OMI data overestimate ground based erythemally weighted UV irradiances retrieved from both Brewer and YES Radiometer (biases about 20%). The effect of aerosols on UV comparisons was investigated in terms of Aerosol Optical Depth (AOD), showing medium-large correlation at SZA larger than 55°. Further sources of uncertainty, such as the difference in the atmospheric conditions between local noon and OMI overpass time and the OMI spatial resolution, were also discussed.
Impacts of climate change on air pollution levels in the Northern Hemisphere with special focus on Europe and the Arctic
Authors: Hedegaard G. B. , Brandt J. , Christensen J. H. , Frohn L. M. , Geels C. , Hansen K. M. , Stendel M.
Published: April 2010

Abstract. The response of a selected number of chemical species is inspected with respect to climate change. The coupled Atmosphere-Ocean General Circulation Model ECHAM4-OPYC3 is providing meteorological fields for the Chemical long-range Transport Model DEHM. Three selected decades (1990s, 2040s and 2090s) are inspected. The 1990s are used as a reference and validation period. In this decade an evaluation of the output from the DEHM model with ECHAM4-OPYC3 meteorology input data is carried out. The model results are tested against similar model simulations with MM5 meteorology and against observations from the EMEP monitoring sites in Europe. The test results from the validation period show that the overall statistics (e.g. mean values and standard deviations) are similar for the two simulations. However, as one would expect the model setup with climate input data fails to predict correctly the timing of the variability in the observations. The overall performance of the ECHAM4-OPYC3 setup as meteorological input to the DEHM model is shown to be acceptable according to the applied ranking method. It is concluded that running a chemical long-range transport model on data from a "free run" climate model is scientifically sound. From the model runs of the three decades, it is found that the overall trend detected in the evolution of the chemical species, is the same between the 1990 decade and the 2040 decade and between the 2040 decade and the 2090 decade, respectively. The dominating impacts from climate change on a large number of the chemical species are related to the predicted temperature increase. Throughout the 21th century the ECHAM4-OPYC3 projects a global mean temperature increase of 3 K with local maxima up to 11 K in the Arctic winter based on the IPCC A2 emission scenario. As a consequence of this temperature increase, the temperature dependent biogenic emission of isoprene is predicted to increase significantly over land by the DEHM model. This leads to an increase in the O3 production and together with an increase in water vapor to an increase in the number of free OH radicals. Furthermore this increase in the number of OH radicals contributes to a significant change in the typical life time of many species, since OH are participating in a large number of chemical reactions. It is e.g. found that more SO42− will be present in the future over the already polluted areas and this increase can be explained by an enhanced conversion of SO2 to SO42−.
Technical Note: Validation of Odin/SMR limb observations of ozone, comparisons with OSIRIS, POAM III, ground-based and balloon-borne instruments
Authors: Jégou F. , Urban J. , de La Noë J. , Ricaud P. , Le Flochmoën E. , Murtagh D. P. , Eriksson P. , Jones A. , Petelina S. , Llewellyn E. J. , Lloyd N. D. , Haley C. , Lumpe J. , Randall C. , Bevilacqua R. M. , Catoire V. , Huret N. , Berthet G. , Renard J. B. , Strong K. , Davies J. , Mc Elroy C. T. , Goutail F. , Pommereau J. P.
Published: April 2010

Abstract. The Odin satellite carries two instruments capable of determining stratospheric ozone profiles by limb sounding: the Sub-Millimetre Radiometer (SMR) and the UV-visible spectrograph of the OSIRIS (Optical Spectrograph and InfraRed Imager System) instrument. A large number of ozone profiles measurements were performed during six years from November 2001 to present. This ozone dataset is here used to make quantitative comparisons with satellite measurements in order to assess the quality of the Odin/SMR ozone measurements. In a first step, we compare Swedish SMR retrievals version 2.1, French SMR ozone retrievals version 222 (both from the 501.8 GHz band), and the OSIRIS retrievals version 3.0, with the operational version 4.0 ozone product from POAM III (Polar Ozone Atmospheric Measurement). In a second step, we refine the Odin/SMR validation by comparisons with ground-based instruments and balloon-borne observations. We use observations carried out within the framework of the Network for Detection of Atmospheric Composition Change (NDACC) and balloon flight missions conducted by the Canadian Space Agency (CSA), the Laboratoire de Physique et de Chimie de l\\'{}Environnement (LPCE, Orléans, France), and the Service d'Aéronomie (SA, Paris, France). Coincidence criteria were 5° in latitude×10° in longitude, and 5 h in time in Odin/POAM III comparisons, 12 h in Odin/NDACC comparisons, and 72 h in Odin/balloons comparisons. An agreement is found with the POAM III experiment (10–60 km) within −0.3±0.2 ppmv (bias±standard deviation) for SMR (v222, v2.1) and within −0.5±0.2 ppmv for OSIRIS (v3.0). Odin ozone mixing ratio products are systematically slightly lower than the POAM III data and show an ozone maximum lower by 1–5 km in altitude. The comparisons with the NDACC data (10–34 km for ozonesonde, 10–50 km for lidar, 10–60 for microwave instruments) yield a good agreement within −0.15±0.3 ppmv for the SMR data and −0.3±0.3 ppmv for the OSIRIS data. Finally the comparisons with instruments on large balloons (10–31 km) show a good agreement, within −0.7±1 ppmv. The official SMR v2.1 dataset is consistent in all altitude ranges with POAM III, NDACC and large balloon-borne instruments measurements. In the SMR v2.1 data, no different systematic error has been found in the 0–35km range in comparison with the 35–60 km range. The same feature has been highlighted in both hemispheres in SMR v2.1/POAM III intercomparisons, and no latitudinal dependence has been revealed in SMR v2.1/NDACC intercomparisons.
Quantification of transport across the boundary of the lower stratospheric vortex during Arctic winter 2002/2003
Authors: Günther G. , Müller R. , von Hobe M. , Stroh F. , Konopka P. , Volk C. M.
Published: April 2010

Abstract. Strong perturbations of the Arctic stratosphere during the winter 2002/2003 by planetary waves led to enhanced stretching and folding of the vortex. On two occasions the vortex in the lower stratosphere split into two secondary vortices that re-merged after some days. As a result of these strong disturbances the role of transport in and out of the vortex was stronger than usual. An advection and mixing simulation with the Chemical Lagrangian Model of the Stratosphere (CLaMS) utilising a suite of inert tracers tagging the original position of the air masses has been carried out. The results show a variety of synoptic and small scale features in the vicinity of the vortex boundary, especially long filaments peeling off the vortex edge and being slowly mixed into the mid latitude environment. The vortex folding events, followed by re-merging of different parts of the vortex led to strong filamentation of the vortex interior. During January, February, and March 2003 flights of the Russian high-altitude aircraft Geophysica were performed in order to probe the vortex, filaments and in one case the merging zone between the secondary vortices. Comparisons between CLaMS results and observations obtained from the Geophysica flights show in general good agreement. Several areas affected by both transport and strong mixing could be identified, allowing explanation of many of the structures observed during the flights. Furthermore, the CLaMS simulations allow for a quantification of the air mass exchange between mid latitudes and the vortex interior. The simulation suggests that after the formation of the vortex was completed, its interior remaind relatively undisturbed. Only during the two re-merging events were substantial amounts of extra-vortex air transported into the polar vortex. When in March the vortex starts weakening additional influence from lower latitudes becomes apparent in the model results. In the lower stratosphere export of vortex air leads only to a fraction of about 5% polar air in mid latitudes by the end of March. An upper limit for the contribution of ozone depleted vortex air on mid-latitude ozone loss is derived, indicating that the maximum final impact of dilution is on the order of 50%.
Seasonal and inter-annual variations in troposphere-to-stratosphere transport from the tropical tropopause layer
Authors: Levine J. G. , Braesicke P. , Harris N. R. P. , Pyle J. A.
Published: April 2010

Abstract. In an earlier study of troposphere-to-stratosphere transport (TST) via the tropical tropopause layer (TTL), we found that the vast majority of air parcels undergoing TST from the base of the TTL enter the extratropical lowermost stratosphere quasi-horizontally and show little or no regional preference with regards to origin in the TTL or entry into the stratosphere. We have since repeated the trajectory calculations – originally limited to a single Northern Hemisphere winter period – in a variety of months and years to assess how robust our earlier findings are to change of timing. To first order, we find that the main conclusions hold, irrespective of the season, year and phase of the El Niño Southern Oscillation (ENSO). We also explore: the distribution of TST between the Northern and Southern Hemispheres; the sensitivity of modelled TST to the definition of the tropopause; and the routes by which air parcels undergo transport exclusively to the stratospheric overworld. Subject to a dynamical definition of the tropopause, we identify a strong bias towards TST in the Southern Hemisphere, particularly during the Northern Hemisphere summer. The thermal tropopause, defined according to the World Meteorological Organization, lies above the dynamical tropopause throughout the extratropics. Inevitably, on switching to the thermal definition, we calculate much less transport across the tropopause, particularly in the subtropics, which could be important with regards to interpretation of processes affecting ozone chemistry in the extratropical lowermost stratosphere (ELS). In contrast to the rather homogeneous nature of TST into the ELS, we find that transport to the overworld takes place from relatively well-defined regions of the TTL, predominantly above the West Pacific and Indonesia, except for an El Niño period in which most transport takes place from regions above the East Pacific and South America.
Source-receptor relationships between East Asian sulfur dioxide emissions and Northern Hemisphere sulfate concentrations
Authors: Liu J. , Mauzerall D. L. , Horowitz L. W.
Published: April 2010

Abstract. We analyze the effect of varying East Asian (EA) sulfur emissions on sulfate concentrations in the Northern Hemisphere, using a global coupled oxidant-aerosol model (MOZART-2). We conduct a base and five sensitivity simulations, in which sulfur emissions from each continent are tagged, to establish the source-receptor (S-R) relationship between EA sulfur emissions and sulfate concentrations over source and downwind regions. We find that from west to east across the North Pacific, EA sulfate contributes approximately 80%–20% of sulfate at the surface, but at least 50% at 500 hPa. Surface sulfate concentrations are dominated by local anthropogenic sources. Of the sulfate produced from sources other than local anthropogenic emissions (defined here as "background" sulfate), EA sources account for approximately 30%–50% (over the Western US) and 10%–20% (over the Eastern US). The surface concentrations of sulfate from EA sources over the Western US are highest in MAM (up to 0.15 μg/m3), and lowest in DJF (less than 0.06 μg/m3). Reducing EA SO2 emissions will significantly decrease the spatial extent of the EA sulfate influence (represented by the areas where at least 0.1 μg m−3 of sulfate originates from EA) over the North Pacific both at the surface and at 500 hPa in all seasons, but the extent of influence is insensitive to emission increases, particularly in DJF and JJA. We find that EA sulfate concentrations over most downwind regions respond nearly linearly to changes in EA SO2 emissions, but sulfate concentrations over the EA source region increase more slowly than SO2 emissions, particularly at the surface and in winter, due to limited availability of oxidants (in particular of H2O2, which oxidizes SO2 to sulfate in the aqueous phase). We find that similar estimates of the S-R relationship for trans-Pacific transport of EA sulfate would be obtained using either sensitivity (i.e., varying emissions from a region to examine the effects on downwind concentrations) or tagging techniques. Our findings suggest that future changes in EA sulfur emissions may cause little change in the sulfate-induced health impact over downwind continents. However, SO2 emission reductions may significantly reduce the sulfate concentrations and the resulting negative radiative forcing over the North Pacific and the United States, thus providing a warming tendency.
On the volatility and production mechanisms of newly formed nitrate and water soluble organic aerosol in Mexico City
Authors: Hennigan C. J. , Sullivan A. P. , Fountoukis C. I. , Nenes A. , Hecobian A. , Vargas O. , Peltier R. E. , Case Hanks A. T. , Huey L. G. , Lefer B. L. , Russell A. G. , Weber R. J.
Published: April 2010

Abstract. Measurements of atmospheric gases and fine particle chemistry were made in the Mexico City Metropolitan Area (MCMA) at a site ~30 km down wind of the city center. Ammonium nitrate (NH4NO3) dominated the inorganic aerosol fraction and showed a distinct diurnal signature characterized by rapid morning production and a rapid mid-day concentration decrease. Between the hours of 08:00–12:45, particulate water-soluble organic carbon (WSOC) concentrations increased and decreased in a manner consistent with that of NO3−, and the two were highly correlated (R2=0.88) during this time. A box model was used to analyze these behaviors and showed that, for both NO3− and WSOC, the concentration increase was caused primarily (~75–85%) by secondary formation, with a smaller contribution (~15–25%) from the entrainment of air from the free troposphere. For NO3−, a majority (~60%) of the midday concentration decrease was caused by dilution from boundary layer expansion, though a significant fraction (~40%) of the NO3− loss was due to particle evaporation. The WSOC concentration decrease was due largely to dilution (~75%), but volatilization did have a meaningful impact (~25%) on the decrease, as well. The results provide an estimate of ambient SOA evaporation losses and suggest that a significant fraction (~35%) of the fresh MCMA secondary organic aerosol (SOA) measured at the surface volatilized.
Estimation of the vertical profile of sulfur dioxide injection into the atmosphere by a volcanic eruption using satellite column measurements and inverse transport modeling
Authors: Eckhardt S. , Prata A. J. , Seibert P. , Stebel K. , Stohl A.
Published: April 2010

Abstract. An analytical inversion method has been developed to estimate the vertical profile of SO2 emissions from volcanic eruptions. The method uses satellite-observed total SO2 columns and an atmospheric transport model (FLEXPART) to exploit the fact that winds change with altitude – thus, the position and shape of the volcanic plume bear information on its emission altitude. The method finds the vertical emission distribution which minimizes the total difference between simulated and observed SO2 columns while also considering a priori information. We have tested the method with the eruption of Jebel at Tair, Yemen, on 30 September 2007 for which a comprehensive observational data set from various satellite instruments (AIRS, OMI, SEVIRI, CALIPSO) is available. Using satellite data from the first 24 h after the eruption for the inversion, we found an emission maximum near 16 km above sea level (a.s.l.), and secondary maxima near 5, 9, 12 and 14 km a.s.l. 60% of the emission occurred above the tropopause. The emission profile obtained in the inversion was then used to simulate the transport of the plume over the following week. The modeled plume agrees very well with SO2 total columns observed by OMI, and its altitude agrees with CALIPSO aerosol observations to within 1–2 km. The inversion result is robust against various changes in both the a priori and the observations. Even when using only SEVIRI data from the first 15 h after the eruption, the emission profile was reasonably well estimated. The method is computationally very fast. It is therefore suitable for implementation within an operational environment, such as the Volcanic Ash Advisory Centers, to predict the threat posed by volcanic ash for air traffic. It could also be helpful for assessing the sulfur input into the stratosphere, be it in the context of volcanic processes or also for proposed geo-engineering techniques to counteract global warming.
CCN activity and droplet growth kinetics of fresh and aged monoterpene secondary organic aerosol
Authors: Engelhart G. J. , Asa-Awuku A. , Nenes A. , Pandis S. N.
Published: April 2010

Abstract. The ability of secondary organic aerosol (SOA) produced from the ozonolysis of α-pinene and monoterpene mixtures (α-pinene, β-pinene, limonene and 3-carene) to become cloud droplets was investigated. A static CCN counter and a Scanning Mobility CCN Analyser (a Scanning Mobility Particle Sizer coupled with a Continuous Flow counter) were used for the CCN measurements. Consistent with previous studies monoterpene SOA is quite active and would likely be a good source of cloud condensation nuclei (CCN) in the atmosphere. A decrease in CCN activation diameter for α-pinene SOA of approximately 3 nm hr−1 was observed as the aerosol continued to react with oxidants. Hydroxyl radicals further oxidize the SOA particles thereby enhancing the particle CCN activity with time. The initial concentrations of ozone and monoterpene precursor (for concentrations lower than 40 ppb) do not appear to affect the activity of the resulting SOA. Köhler Theory Analysis (KTA) is used to infer the molar mass of the SOA sampled online and offline from atomized filter samples. The estimated average molar mass of online SOA was determined to be 180±55 g mol−1 (consistent with existing SOA speciation studies) assuming complete solubility. KTA suggests that the aged aerosol (both from α-pinene and the mixed monoterpene oxidation) is primarily water-soluble (around 65%). CCN activity measurements of the SOA mixed with (NH4)2SO4 suggest that the organic can depress surface tension by as much as 10 N m−1 (with respect to pure water). The droplet growth kinetics of SOA samples are similar to (NH4)2SO4, except at low supersaturation, where SOA tends to grow more slowly. The CCN activation diameter of α-pinene and mixed monoterpene SOA can be modelled to within 10–15% of experiments by a simple implementation of Köhler theory, assuming complete dissolution of the particles, no dissociation into ions, a molecular weight of 180 g mol−1, a density of 1.5 g cm−3, and the surface tension of water.
Probing ETEX-II data set with inverse modelling
Authors: Krysta M. , Bocquet M. , Brandt J.
Published: April 2010

Abstract. We give here an account on the results of source inversion of the ETEX-II experiment. Inversion has been performed with the maximum entropy method on the basis of non-zero measurements and in conjunction with a transport model POLAIR3D. The discrepancy scaling factor between the reconstructed and the true mass has been estimated to be equal to 7. The results contrast with the method's performance on the ETEX-I source. In the latter case its mass has been reconstructed with an accuracy exceeding 80%. The large value of the discrepancy factor for ETEX-II could be ascribed to modelling difficulties, possibly linked not to the transport model itself but rather to the quality of the measurements.
The role of climate and emission changes in future air quality over southern Canada and northern Mexico
Authors: Tagaris E. , Liao K.-J. , Manomaiphiboon K. , He S. , Woo J.-H. , Amar P. , Russell A. G.
Published: April 2010

Abstract. Potential impacts of global climate and emissions changes on regional air quality over southern (western and eastern) Canada and northern Mexico are examined by comparing future summers' (i.e., 2049–2051) average regional O3 and PM2.5 concentrations with historic concentrations (i.e., 2000–2002 summers). Air quality modeling was conducted using CMAQ and meteorology downscaled from the GISS-GCM using MM5. Emissions for North America are found using US EPA, Mexican and Canadian inventories and projected emissions following CAIR and IPCC A1B emissions scenario. Higher temperatures for all sub-regions and regional changes in mixing height, insolation and precipitation are forecast in the 2049-2051 period. Future emissions are calculated to be lower over both Canadian sub-regions, but higher over northern Mexico. Global climate change, alone, is predicted to affect PM2.5 concentrations more than O3 for the projections used in this study: average daily maximum eight (8) hour O3 (M8hO3) concentrations are estimated to be slightly different in all examined sub-regions while average PM2.5 concentrations are estimated to be higher over both Canadian sub-regions (8% over western and 3% over eastern) but 11% lower over northern Mexico. More days are forecast where M8hO3 concentrations are over 75 ppb in all examined sub-regions but the number of days where PM2.5 concentration will be over 15 μg/m3 is projected higher only over western Canada. Climate change combined with the projected emissions lead to greater change in pollutant concentrations: average M8hO3 concentrations are simulated to be 6% lower over western Canada and 8% lower over eastern Canada while average PM2.5 concentrations are simulated to be 5% lower over western Canada and 11% lower over eastern Canada. Although future emissions over northern Mexico are projected higher, pollutant concentrations are simulated to be lower due to US emissions reductions. Global climate change combined with the projected emissions will decrease average M8hO3 4% and PM2.5 17% over northern Mexico. Significant reductions in the number of days where M8hO3 concentrations are over 75 ppb and PM2.5 concentration over 15 μg/m3 are also projected with a significant reduction in peak values.
Error analysis for CO and CH4 total column retrievals from SCIAMACHY 2.3 μm spectra
Authors: Gloudemans A. M. S. , Schrijver H. , Hasekamp O. P. , Aben I.
Published: April 2010

Abstract. A detailed sensitivity analysis of the Iterative Maximum Likelihood Method (IMLM) algorithm and its application to the SCIAMACHY 2.3 μm spectra is presented. The sensitivity analysis includes a detailed assessment of the impact of aerosols in the 2.3 μm range. Results show that near strong aerosol sources mineral dust and biomass aerosols can have an effect of ~7–10% on the CH4 total columns retrieved from this wavelength range if aerosol scattering is neglected in the retrieval algorithm. Similar but somewhat larger effects are found for CO, but due to the larger variability of CO these errors are less important. Away from strong sources much smaller effects of a few percent are found. Using CH4 as a proxy for CO and/or including aerosol information in the retrieval algorithm significantly reduces these errors for both CO and CH4. Spectroscopic uncertainties are mostly negligible except for uncertainties in the CH4 intrinsic line intensities, which can be important. Application of the IMLM algorithm to the SCIAMACHY 2.3 μm spectra shows that the quality of the retrieved CO and CH4 total columns is good, except for a bias for large instrument-noise errors which is partly due to remaining calibration issues. Polarization sensitivity of the SCIAMACHY instrument has a negligible effect on the retrieved CO and CH4 total columns. The H2O total columns, which have to be retrieved simultaneously with CO and CH4 due to overlapping absorption lines, agree well with H2O total columns from ECMWF data. This ensures that the fit to the H2O absorptions is of sufficient quality not to hamper the retrieved CO and CH4 total columns from SCIAMACHY spectra.
Fast airborne aerosol size and chemistry measurements above Mexico City and Central Mexico during the MILAGRO campaign
Authors: DeCarlo P. F. , Dunlea E. J. , Kimmel J. R. , Aiken A. C. , Sueper D. , Crounse J. , Wennberg P. O. , Emmons L. , Shinozuka Y. , Clarke A. , Zhou J. , Tomlinson J. , Collins D. R. , Knapp D. , Weinheimer A. J. , Montzka D. D. , Campos T. , Jimenez J. L.
Published: April 2010

Abstract. The concentration, size, and composition of non-refractory submicron aerosol (NR-PM1) was measured over Mexico City and central Mexico with a High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) onboard the NSF/NCAR C-130 aircraft as part of the MILAGRO field campaign. This was the first aircraft deployment of the HR-ToF-AMS. During the campaign the instrument performed very well, and provided 12 s data. The aerosol mass from the AMS correlates strongly with other aerosol measurements on board the aircraft. Organic aerosol (OA) species dominate the NR-PM1 mass. OA correlates strongly with CO and HCN indicating that pollution (mostly secondary OA, SOA) and biomass burning (BB) are the main OA sources. The OA to CO ratio indicates a typical value for aged air of around 80 μg m−3 (STP) ppm−1. This is within the range observed in outflow from the Northeastern US, which could be due to a compensating effect between higher BB but lower biogenic VOC emissions during this study. The O/C atomic ratio for OA is calculated from the HR mass spectra and shows a clear increase with photochemical age, as SOA forms rapidly and quickly overwhelms primary urban OA, consistent with Volkamer et al. (2006) and Kleinman et al. (2008). The stability of the OA/CO while O/C increases with photochemical age implies a net loss of carbon from the OA. BB OA is marked by signals at m/z 60 and 73, and also by a signal enhancement at large m/z indicative of larger molecules or more resistance to fragmentation. The main inorganic components show different spatial patterns and size distributions. Sulfate is regional in nature with clear volcanic and petrochemical/power plant sources, while the urban area is not a major regional source for this species. Nitrate is enhanced significantly in the urban area and immediate outflow, and is strongly correlated with CO indicating a strong urban source. The importance of nitrate decreases with distance from the city likely due to evaporation. BB does not appear to be a strong source of nitrate despite its high emissions of nitrogen oxides, presumably due to low ammonia emissions. NR-chloride often correlates with HCN indicating a fire source, although other sources likely contribute as well. This is the first aircraft study of the regional evolution of aerosol chemistry from a tropical megacity.
Amines are likely to enhance neutral and ion-induced sulfuric acid-water nucleation in the atmosphere more effectively than ammonia
Authors: Kurtén T. , Loukonen V. , Vehkamäki H. , Kulmala M.
Published: April 2010

Abstract. We have studied the structure and formation thermodynamics of dimer clusters containing H2SO4 or HSO4− together with ammonia and seven different amines possibly present in the atmosphere, using the high-level ab initio methods RI-MP2 and RI-CC2. As expected from e.g. proton affinity data, the binding of all studied amine-H2SO4 complexes is significantly stronger than that of NH3•H2SO4, while most amine-HSO4− complexes are only somewhat more strongly bound than NH3•HSO4−. Further calculations on larger cluster structures containing dimethylamine or ammonia together with two H2SO4 molecules or one H2SO4 molecule and one HSO4− ion demonstrate that amines, unlike ammonia, significantly assist the growth of not only neutral but also ionic clusters along the H2SO4 co-ordinate. A sensitivity analysis indicates that the difference in complexation free energies for amine- and ammonia-containing clusters is large enough to overcome the mass-balance effect caused by the fact that the concentration of amines in the atmosphere is probably 2 or 3 orders of magnitude lower than that of ammonia. This implies that amines might be more important than ammonia in enhancing neutral and especially ion-induced sulfuric acid-water nucleation in the atmosphere.
Evaluated kinetic and photochemical data for atmospheric chemistry: Volume IV – gas phase reactions of organic halogen species
Authors: Atkinson R. , Baulch D. L. , Cox R. A. , Crowley J. N. , Hampson R. F. , Hynes R. G. , Jenkin M. E. , Rossi M. J. , Troe J. , Wallington T. J.
Published: April 2010

Abstract. This article, the fourth in the series, presents kinetic and photochemical data sheets evaluated by the IUPAC Subcommittee on Gas Kinetic Data Evaluation for Atmospheric Chemistry. It covers the gas phase and photochemical reactions of organic halogen species, which were last published in 1997, and were updated on the IUPAC website in 2006/07. The article consists of a summary sheet, containing the recommended kinetic parameters for the evaluated reactions, and four appendices containing the data sheets, which provide information upon which the recommendations are made.
Impacts of the solar eclipse of 29 March 2006 on the surface ozone concentration, the solar ultraviolet radiation and the meteorological parameters at Athens, Greece
Authors: Tzanis C. , Varotsos C. , Viras L.
Published: April 2010

Abstract. In this study the variations in the surface ozone concentration, the solar ultraviolet radiation and the meteorological parameters at the ground before, during and after the total solar eclipse of 29 March 2006 have been examined. This analysis is based on the measurements performed at four stations located in the greater Athens basin in Greece. The experimental data demonstrated that the solar eclipse phenomenon affects the surface ozone concentration as well as the temperature, the relative humidity and the wind speed near the ground. The decrease in the surface ozone concentration that observed after the beginning of the eclipse event lasted almost two hours, probably due to the decreased efficiency of the photochemical ozone formation. The reduction of the solar ultraviolet radiation at 312 and 365 nm reached 97% and 93% respectively, while the air temperature dropped, the relative humidity increased and the wind speed decreased.
Evaluation of a new lightning-produced NOx parameterization for cloud resolving models and its associated uncertainties
Authors: Barthe C. , Barth M. C.
Published: April 2010

Abstract. A new parameterization of the lightning-produced NOx has been developed for cloud-resolving models. This parameterization is based on the unique characteristics of identifying which convective cells are capable of producing lightning based on a vertical velocity threshold and estimating the lightning flash rate in each convective cell from the non-precipitation and precipitation ice mass flux product. Further, the source location is filamentary instead of volumetric as in most previous parameterizations. This parameterization has been tested on the 10 July 1996 Stratospheric-Tropospheric Experiment: Radiation, Aerosols and Ozone (STERAO) storm. Comparisons of the simulated flash rate and NO mixing ratio (control experiment) with observations at different locations and stages of the storm show good agreement. An individual flash produces on average 121±41 moles of NO (7.3±2.5×1025 molecules NO) for the simulated high cloud base, high shear storm that is dominated by intra-cloud flash activity. Sensitivity tests have been performed to study the impact of the flash rate, the cloud-to-ground flash ratio, the flash length, the spatial distribution of the NO molecules, and the production rate per flash on the NO concentration and distribution. Results show a strong impact from the flash rate, the spatial placement of the lightning-NOx source and the number of moles produced per flash. On the other hand, the simulations show almost no impact from the different cloud-to-ground (CG) ratios and the lightning-NOx production rates per CG flash used as input to the model.