Understanding the contributions of anthropogenic and biogenic sources to CO enhancements and outflow observed over North America and the western Atlantic Ocean by TES and MOPITT

We investigate the effects of anthropogenic and biogenic sources on tropospheric CO enhancements and outflow over North America and the Atlantic during July–August 2006, the 3rd warmest summer on record. The analysis is performed using the 3D Regional chEmical trAnsport Model (REAM), satellite data from TES on the Aura satellite, MOPITT on the Terra satellite and surface monitor data from the SEARCH network. The satellite measurements of CO provide insight into the location of regional CO enhancements along with the ability to resolve vertical features. Satellite and surface monitor data are used to compare with REAM, illustrating model's ability to reproduce observed CO concentrations. The REAM model used in this study features CO emissions reduced by 50% from the 1999 EPA NEI and biogenic VOC emissions scaled by EPA-observed isoprene concentrations (20% reduction). The REAM simulations show large variations in surface CO, lower tropospheric CO and column CO, which are also observed by the surface observations and satellite data. Over the US, during July–August 2006, the model estimates monthly CO production from anthropogenic sources (5.3 and 5.1 Tg CO) is generally larger than biogenic sources (4.3 and 3.5 Tg CO). However, the model shows that for very warm days, biogenic sources produce as much CO as anthropogenic sources, a result of increased biogenic production due to warmer temperatures. The satellite data show CO outflow occurs along the East Coast of the US and Canada in July and is more broadly distributed over the Atlantic in August. REAM results show the longitudinally exported CO enhancements from anthropogenic sources (3.3 and 3.9 Tg CO) are larger than biogenic sources (2.8 and 2.7 Tg CO) along the eastern boundary of REAM for July–August 2006. We show that when compared with the impacts of both sources on increasing tropospheric CO exports, the relative impacts in August are greater than in July because of preferable outflow transport.     

Seasonal trends,meteorological impacts,and associated health risks with atmospheric concentrations of gaseous pollutants at an Indian coastal city

This study presents surface ozone (O₃) and carbon monoxide (CO) measurements conducted at Bhubaneswar from December 2010 to November 2012 and attempts for the very first time a health risk assessment of the atmospheric trace gases. Seasonal variation in average 24 h O₃ and CO shows a distinct winter (December to February) maxima of 38.98?±?9.32 and 604.51?±?145.91 ppbv, respectively. O₃ and CO characteristics and their distribution were studied in the form of seasonal/diurnal variations, air flow patterns, inversion conditions, and meteorological parameters. The observed winter high is likely due to higher regional emissions, the presence of a shallower boundary layer, and long-range transport of pollutants from the Indo-Gangetic Plain (IGP). Large differences between daytime and nighttime O₃ values during winter compared to other seasons suggest that photochemistry is much more active on this site during winter. O₃ and CO observations are classified in continental and marine air masses, and continental influence is estimated to increase O₃ and CO by up to 20 and 120 ppbv, respectively. Correlation studies between O₃ and CO in various seasons indicated the role of CO as one of the O₃ precursors. Health risk estimates predict 48 cases of total premature mortality in adults due to ambient tropospheric O₃ during the study period. Comparatively low CO concentrations at the site do not lead to any health effects even during winter. This study highlights the possible health risks associated with O₃ and CO pollution in Bhubaneswar, but these results are derived from point measurements and should be complemented either with regional scale observations or chemical transport models for use in design of mitigation policies.     

Lightning-tropospheric ozone connections: EOF analysis of TCO and lightning data

An empirical orthogonal function (EOF) analysis is applied to two different data sets of tropospheric column ozone (TCO) and observed lightning flash rates over the tropical Atlantic for the period of 1996–2000. The first two dominant EOF modes of TCO values, explaining more than 65% of total variance are characterized by the seasonal cycle. The time series of EOF1 and EOF2 of TCO values are in phase with those of the EOF2 (16%) and EOF1 (63%) of the lightning, respectively. These relationships imply the influence of lightning on the tropical ozone maximum and the tropical ozone paradox. Moreover, the spatial distribution of the EOF modes and the horizontal wind field in the upper troposphere show that the highest lightning flash rates are located upstream of the region where high TCO values are found throughout the year.     

The Greenhouse effect: impacts of ultraviolet-B (UV-B) radiation, carbon dioxide (CO2), and ozone (O3) on vegetation

There is a fast growing and an extremely serious international scientific, public and political concern regarding man's influence on the global climate. The decrease in stratospheric ozone (O3) and the consequent possible increase in ultraviolet-B (UV-B) is a critical issue. In addition, tropospheric concentrations of 'greenhouse gases' such as carbon dioxide (CO2), nitrous oxide (N2O) and methane (CH4) are increasing. These phenomena, coupled with man's use of chlorofluorocarbons (CFCs), chlorocarbons (CCs), and organo-bromines (OBs) are considered to result in the modification of the earth's O3 column and altered interactions between the stratosphere and the troposphere. A result of such interactions could be the global warming. As opposed to these processes, tropospheric O3 concentrations appear to be increasing in some parts of the world (e.g. North America). Such tropospheric increases in O3 and particulate matter may offset any predicted increases in UV-B at those locations. Presently most general circulation models (GCMs) used to predict climate change are one- or two-dimensional models. Application of satisfactory three-dimensional models is limited by the available computer power. Recent studies on radiative cloud forcing show that clouds may have an excess cooling effect to compensate for a doubling of global CO2 concentrations. There is a great deal of geographic patchiness or variability in climate. Use of global level average values fails to account for this variability. For example, in North America: 1. there may be a decrease in the stratospheric O3 column (1-3%); however, there appears to be an increase in tropospheric O3 concentrations (1-2%/year) to compensate up to 20-30% loss in the total O3 column; 2. there appears to be an increase in tropospheric CO2, N2O and CH4 at the rate of roughly 0.8%, 0.3% and 1-2%, respectively, per year; 3. there is a decrease in erythemal UV-B; and 4. there is a cooling of tropospheric air temperature due to radiative cloud forcing. The effects of UV-B, CO2 and O3 on plants have been studied under growth chamber, greenhouse and field conditions. Few studies, if any, have examined the joint effects of more than one variable on plant response. There are methodological problems associated with many of these experiments. Thus, while results obtained from these studies can assist in our understanding, they must be viewed with caution in the context of the real world and predictions into the future. Biomass responses of plants to enhanced UV-B can be negative (adverse effect); positive (stimulatory effect) or no effect (tolerant). Sensitivity rankings have been developed for both crop and tree species. However, such rankings for UV-B do not consider dose-response curves. There are inconsistencies between the results obtained under controlled conditions versus field observations. Some of these inconsistencies appear due to the differences in responses between cultivars and varieties of a given plant species; and differences in the experimental methodology and protocol used. Nevertheless, based on the available literature, listings of sensitive crop and native plant species to UV-B are provided. Historically, plant biologists have studied the effects of CO2 on plants for many decades. Experiments have been performed under growth chamber, greenhouse and field conditions. Evidence is presented for various plant species in the form of relative yield increases due to CO2 enrichment. Sensitivity rankings (biomass response) are agein provided for crops and native plant species. However, most publications on the numerical analysis of cause-effect relationships do not consider sensitivity analysis of the mode used. Ozone is considered to be the most phytotoxic regional scale air pollutant. In the pre-occupation of loss in the O3 column, any increases in tropospheric O3 concentrations may be undermined relative to vegetation effects. As with the other stress factors, the effects of O3 have been studied both under controlled and field conditions. Thboth under controlled and field conditions. The numerical explanation of cause-effect relationships of O3 is a much debated subject at the present time. Much of the controversy is directed toward the definition of the highly stochastic, O3 exposure dynamics in time and space. Nevertheless, sensitivity rankings (biomass response) are provided for crops and native vegetation. The joint effects of UV-B, CO2 and O3 are poorly understood. Based on the literature of plant response to individual stress factors and chemical and physical climatology of North America, we conclude that nine different crops may be sensitive to the joint effects: three grain and six vegetable crops (sorghum, oat, rice, pea, bean, potato, lettuce, cucumber and tomato). In North America, we consider Ponderosa and loblolly pines as vulnerable among tree species. This conclusion should be moderated by the fact that there are few, if any, data on hardwood species. In conclusion there is much concern for global climate change and its possible effects on vegetation. While this is necessary, such a concern and any predictions must be tempered by the lack of sufficient knowledge. Experiments must be designed on an integrated and realistic basis to answer the question more definitively. This would require very close co-operation and communication among scientists from multiple disciplines. Decision makers must realize this need.     

The impact of transpacific transport of mineral dust in the United States

We use a global chemical transport model (GEOS-Chem) to estimate the impact of transpacific transport of mineral dust on aerosol concentrations in North America during 2001. We have implemented two dust mobilization schemes in the model (GOCART and DEAD) and find that the best simulation of North American surface observations with GEOS-Chem is achieved by combining the topographic source used in GOCART with the entrainment scheme used in DEAD. This combination restricts dust emissions to year-round arid areas but includes a significant wind threshold for dust mobilization. The model captures the magnitude and seasonal cycle of observed surface dust concentrations over the northern Pacific. It simulates the free tropospheric outflow of dust from Asia observed in the TRACE-P and ACE-Asia aircraft campaigns of spring 2001. It reproduces the timing and distribution of Asian dust outbreaks in North America during April–May. Beyond these outbreaks we find persistent Asian fine dust (averaging 1.2 μg m⁻³) in surface air over the western United States in spring, with much weaker influence (0.25 μg m⁻³) in summer and fall. Asian influence over the eastern United States is 30–50% lower. We find that transpacific sources accounted for 41% of the worst dust days in the western United States in 2001.     

The impact of natural and anthropogenic hydrocarbons on the tropospheric budget of carbon monoxide

A method to quantify the relative contributions of surface sources and photochemical production of atmospheric carbon monoxide has been implemented in a three-dimensional chemical-transport model. The impact of biogenic and anthropogenic hydrocarbons has been calculated. The oxidation of isoprene contributes to about 10% of the global tropospheric burden of carbon monoxide, with a maximum contribution over southern America and Africa. Oxidation of methane and terpenes contribute to 28 and 2%, respectively, of the tropospheric burden of CO. The oxidation of the other hydrocarbons, which include ethane, propane, ethylene, propylene and the surrogate hydrocarbon representing other hydrocarbons results in 12% of the CO tropospheric burden, among which 69% results from the oxidation of hydrocarbons of biologic origin. The overall global CO yield from the oxidation of isoprene is estimated to be 23% on a carbon basis. Comparisons between model results and the few available observations of isoprene, terpenes and their oxidation products show that there is no evidence that the current global isoprene emissions proposed in the IGAC/GEIA emissions data base are substantially overestimated, as suggested by previous studies.     

Relationships between emission sources and air mass characteristics in East Asia during the TRACE-P period

Long-range transport of pollutants influenced by anthropogenic and natural emission sources in East Asia is investigated by using backward trajectory analysis along the NASA TRACE-P flight tracks and a numerical simulation with the three-dimensional chemical transport model (STEM-2k1). Observation-based regional distributions of trace gases are reconstructed using the observations obtained by measurements on board the DC-8 and P3-B aircrafts. Systematic features of the spatial distribution for each species are identified. It is found that the observed concentrations of CO and some NMHCs, and the ratios between these species, are highly associated with the source distribution features and their regional characteristics. Reconstructed fields of the observed and modeled ethane/CO and ethane/propane are found to reproduce well the estimated emission ratios in East Asia. We also investigated the time rate of change of the concentration of species and their ratio along the trajectory. From this analysis the propane/ethane and propane/acetylene ratios are shown to preserve their emission ratios during regional transport. However systematic differences in the propane vs. acetylene/CO relationships are found between the model and observation values. This analysis suggests that further efforts are needed to improve the estimates of biomass burning emissions in SE Asia. The results presented in this paper also suggest ways to further extend the capabilities to derive observation-based inventories.     

Satellite derived trends in NO2 over the major global hotspot regions during the past decade and their inter-comparison

We assessed satellite derived tropospheric NO₂ distribution on a global scale and identified the major NO₂ hotspot regions. Combined GOME and SCIAMACHY measurements for the period 1996-2006 have been used to compute the trends over these regions. Our analysis shows that tropospheric NO₂ column amounts have increased over the newly and rapidly developing regions like China (11 ± 2.6%/year), south Asia (1.76 ± 1.1%/year), Middle East (2.3 ± 1%/year) and South Africa (2.4 ± 2.2%/year). Tropospheric NO₂ column amounts show some decrease over the eastern US (−2 ± 1.5%/year) and Europe (0.9 ± 2.1%/year). We found that although tropospheric NO₂ column amounts decreased over the major developed regions in the past decade, the present tropospheric NO₂ column amounts over these regions are still significantly higher than those observed over newly and rapidly developing regions (except China). Tropospheric NO₂ column amounts show some decrease over South America and Central Africa, which are major biomass burning regions in the Southern Hemisphere.     

The variability of free tropospheric ozone over Beltsville,Maryland (39N, 77W) in the summers 2004–2007

Ozone profiles are often used to investigate day-to-day and year-to-year variability in origins of free tropospheric ozone. With this in mind, more than 50 ozonesonde launches were conducted in Beltsville, MD, during the summers of 2004 through 2007. Budgets of free tropospheric ozone were calculated for each ozone profile in the four summers using a laminar identification (LID) method and unusual episodes were analyzed with respect to meteorological variables. The laminar method showed that stratosphere-to-troposphere transport (ST) accounted for greater than 50% of the free tropospheric ozone column on 17% of days sampled, a more pronounced influence than regional convective and lightning (RCL) sources. The ST origins were confirmed with trajectories, and tracers (water vapor and potential vorticity). The amount of free tropospheric ozone from ST and RCL sources varied from year-to-year (up to 13%) and can be explained by differences in mean meteorological patterns. On average, almost 30% of the free tropospheric column was attributed to ST influence, about twice as much as RCL, although the LID method may not capture weeks-old lightning influences as in a chemical model. The prevalence of ST ozone in summertime Beltsville soundings was similar to six sounding sites in the IONS-04 campaign [Thompson, A.M., et al., 2007b. Intercontinental Transport Experiment Ozonesonde Network Study (IONS, 2004): 1. Summertime upper tropospheric/lower stratosphere ozone over northeastern North America. J. Geophys. Res. 112, D12S12; Thompson, A.M., et al., 2007c. Intercontinental Transport Experiment Ozonesonde Network Study (IONS, 2004): 2. Tropospheric ozone budgets and variability over northeastern North America. J. Geophys. Res. 112, D12S13.] and to statistics from a 30 year climatology of European soundings [Collette, A., Ancellet, G., 2005. Impact of vertical transport processes on the tropospheric ozone layering above Europe. Part II: Climatological analysis of the past 30 years. Atmos. Environ. 39, 5423–5435]. The Beltsville record also demonstrated the value of soundings for air quality forecasting in an urban area. The 22 nighttime soundings collected over Beltsville in 2004–2007 can be divided into distinct polluted and unpolluted subsets, the former 20 ppbv higher in residual layer ozone (1 km) than the latter. These distinctions propagated to daytime differences of 10 ppbv at the surface in the Washington, DC, area, with the high-ozone residual layers leading to non-attainment of the National Ambient Air Quality Standard for ozone. More frequent ozone observations aloft appear essential for better understanding ozone variability and for enabling air quality modelers to achieve more accurate ozone forecasts.     

Simulation of the tropospheric distribution of carbon monoxide during the 1984 MAPS experiment

A global, three-dimensional tropospheric chemistry model was used to perform simulations of the tropospheric distribution of carbon monoxide (CO) coinciding with NASA's Measurement of Air Pollution from Satellites (MAPS) experiment which took place during 5–13 October 1984. Archived meteorological data for September and October, 1984, were obtained from the European Centre for Medium-Range Weather Forecasting and used to drive the offline chemical transport model simulations. Base-case CO emissions were generated by applying emission factors to compiled inventories for related or co-emitted trace species. Simulation results from September and October have been compared with a recent re-release of the 1984 MAPS data and with in situ correlative data taken during the MAPS mission. Because of unrealistically large spatial variability in N₂O mixing ratios measured concurrently by MAPS, model results were also compared with an adjusted CO data set generated by assuming that errors in N₂O measured mixing ratios were correlated with errors in the MAPS CO data. These comparisons, in conjunction with simulations probing model sensitivities, led to the conclusion that biomass burning CO emissions from central and southern Africa may have been larger during September and October, 1984, than our initial best estimate based on the CO₂ emissions data of Hao et al. (1990. Fire in the Tropical Biota; Ecosystem Processes and Global Challenges. Springer, Berlin, pp. 440–462; 1994. Global Biogeochemical Cycles 8, 495–503). This result is in disagreement with recent estimates of biomass burning emissions from Africa (Scholes et al., 1996, Journal of Geophysical Research 101, 23677–23682) which are smaller than previously thought for emissions from this region. Although unknown model deficiencies cannot be conclusively ruled out, model sensitivity studies indicate that increased CO emissions from central and southern Africa offer the best explanation for reducing observed differences between model results and MAPS data for this time period. Our results, in combination with a disparity in recent CO emission estimates from this region (Scholes et al., 1996; Hao et al., 1996, Journal of Geophysical Research 101, 23577–23584), and in light of recent indications of highly variable biomass burning activities from the tropical western Pacific (Folkins et al., 1997, Journal of Geophysical Research 102, 13291–13299), seem to suggest that biomass burning emissions exhibit significant year-to-year variability. This large variability of emissions sources makes the accurate simulation of specific time periods very difficult and suggests that biomass burning trace species inventories may have to be developed specifically for each simulated time period, employing satellite-derived information on fire coverage and flame intensity.     

Continuous measurement of peroxyacetyl nitrate (PAN) in suburban and remote areas of western China

Knowledge on atmospheric abundance of peroxyacetyl nitrate (PAN) is important in assessing the severity of photochemical pollution, and for understanding chemical transformation of reactive odd nitrogen and its impact on the budget of tropospheric ozone (O₃). In summer 2006, continuous measurements of PAN were made using an automatic GC–ECD analyzer with an on-line calibrator at a suburban site of Lanzhou (LZ) and a remote site of Mt. Waliguan (WLG) in western China, with concurrent measurements of O₃, total reactive nitrogen (NO_y) and carbon monoxide (CO). At LZ, several photochemical episodes were observed during the study, and the average mixing ratio of PAN (plus or minus standard deviation) was 0.76 (±0.89) ppbv with the maximum value of 9.13 ppbv, compared to an average value of 0.44 (±0.16) ppbv at remote WLG. The PAN mixing ratios in LZ exhibited strong diurnal variations with a maximum at noon, while enhanced concentrations of PAN were observed in the evening and a minimum in the afternoon at WLG. The daily O₃ and PAN concentration maxima showed a strong correlation (r² = 0.91) in LZ, with a regression slope (PAN/O₃) of 0.091 ppbv ppbv^?1. At WLG, six well-identified pollution plumes (lasting 2–8 h) were observed with elevated concentrations of PAN (and other trace gases), and analysis of backward particle release simulation shows that the high-PAN events at WLG were mostly associated with the transport of air masses that had passed over LZ.     

Monitoring of ozone in a marine environment in Tenerife (Canary Islands)

In the Aguere Valley (in the oceanic boundary layer at Tenerife, 28°N, 16°W, 580 m a.s.l.) the ozone levels were monitored for ambient air quality assessment. Although precursors are emitted in this area, the strong correlation between ozone levels and wind velocity indicates that ozone is transported into the valley from the ocean. The inland ozone supply along the valley is induced by an orographic channelling effect of the northern oceanic air masses. The highest ozone concentrations are mostly recorded during the nocturnal stage under the influence of fresh oceanic air masses, and during high wind speed events. The seasonal cycle is characterised by elevated ozone mixing ratios in the spring (nighttime levels >45 ppbv) and low mixing ratios in the summer (nighttime levels in the range 20–35 ppbv). Back-trajectory analysis shows that the ozone monitored in the Aguere Valley is associated with long-range transport processes. High ozone events in the spring are associated with transport from upper tropospheric levels, both over the North Atlantic-high latitudes (>45°N) and Europe. This downward transport was observed in the western edge of upper tropospheric cyclones, which suggests that the upper tropospheric/low stratospheric ozone sources play a significant role. In summer, ozone is mainly transported from the North Atlantic-high latitudes (>45°N) and from mid- to low-tropospheric levels. In autumn and winter, the high ozone concentrations are transported from sources located a few km above the North Atlantic-high latitudes (>45°N) and over Europe. The Central-North Atlantic (<45°N) and North Africa are not significant sources of ozone. The high spring and lower summer ozone events in the Aguere Valley agree with other North Atlantic ozone observation in the oceanic boundary layer. However, this behaviour contrasts with the high ozone events frequently recorded at Izaña BAPMoN station (located in the free troposphere in Tenerife) during the summer, which have been attributed in the literature to downward transport from upper levels. An intensification of the inversion layer that separates the oceanic boundary layer of the free troposphere during the summer in Canary Islands is interpreted as the cause of this different behaviour between ozone in the Aguere Valley and Izaña BAPMoN station.     

Impact of vertical transport processes on the tropospheric ozone layering above Europe. Part I: Study of air mass origin using multivariate analysis,clustering and trajectories

A new method is proposed to classify ozone-rich layers observed in tropospheric profiles in terms of their origin using multivariate analysis. We combine principal component and discriminant analyses to quantify the respective ability of 21 measured physical parameters to describe the layers. Agglomerative hierarchical clustering shows the existence of clusters of air masses with specific physical characteristics. Quadratic discriminant analysis allows the definition of multidimensional borders between these clusters. The geophysical characteristics of the clusters are discussed and related to the origins of the layers: recently transported from the stratosphere (ST) or from the boundary layer (BL) or transported over long distances in the free troposphere.This clustering is compared to the results of a Lagrangian particle dispersion model for a 2-year period. The proportions of layers originating either from the BL or from the ST are highly consistent using both methods as well as the respective contribution of each reservoir to the total ozone mass. About 10% of the ozone measured in the tropospheric layers was exported recently from the BL and one-fifth has a recent stratospheric origin. The remaining proportion could not be attributed to any recent transport pathway. Season-dependent criteria allow very satisfactory reproduction of the seasonal variability of the layering as seen by the Lagrangian model. Analysis of the geographical origin of BL air masses suggests that the statistical clustering underestimates long-range transport, especially in fall.     

Satellite observations of Mexico City pollution outflow from the Tropospheric Emissions Spectrometer (TES)

Concurrent tropospheric O₃ and CO vertical profiles from the Tropospheric Emission Spectrometer (TES) during the MILAGRO/INTEX-B aircraft campaigns over the Mexico City Metropolitan Area (MCMA) and its surrounding regions were used to examine Mexico City pollution outflow on a regional scale. The pollution outflow from the MCMA occurred predominantly at 600–800 hPa as evident in O₃, CO, and NO_x enhancements in the in situ aircraft observations. TES O₃ and CO are sensitive to the MCMA pollution outflow due to their relatively high sensitivities at 600–800 hPa. We examined O₃, CO, and their correlation at 600–800 hPa from TES retrievals, aircraft measurements, and GEOS-Chem model results. TES captures much of the spatial and day-to-day variability of O₃ seen in the in situ data. TES CO, however, shows much less spatial and day-to-day variability compared with the in situ observations. The ΔO₃/ΔCO slope is significantly higher in the TES data (0.43) than the in situ data (0.28) due partly to the lack of variability in TES CO. Extraordinarily high ΔO₃/ΔCO slope (0.81) from TES observations at 618 hPa over the Eastern U.S. was previously reported by Zhang et al. [Zhang, L., Jacob, D.J., Bowman, K.W., et al., 2006. Ozone–CO correlations determined by the TES satellite instrument in continental outflow regions. Geophys. Res. Lett. 33, L18804. 10.1029/2006GL026399.]. Thus the application of TES CO–O₃ correlation to map continental pollution outflow needs further examination.     

Variations of the increasing trend of tropospheric NO2 over central east China during the past decade

A numerical analysis using a regional chemical transport model (CTM) is presented in comparison with Global Ozone Monitoring Experiment (GOME) and SCanning Imaging Absorption spectroMeter for Atmospheric CHartographY (SCIAMACHY) satellite NO₂ measurements over East Asia from 1996 to 2005 from a climatological perspective. Modeling results agree well with satellite retrievals in geographical distribution patterns, with systematic underestimation of the absolute values. The sharp increase in NO₂ vertical column densities (VCDs) over central east China (CEC) after the year 2000 (14.1–20.5% yr⁻¹ for the satellite observations and 10.8% yr⁻¹ for model simulations) is analyzed quantitatively over different megacity clusters. The distinct emission increase patterns are responsible for the different increase trends observed over the Beijing megacity cluster (BJ), the Yangtze Delta (YD) and other CEC regions. The growth rate of satellite measured and CMAQ-modeled NO₂ VCDs for the YD is much higher than that in other regions, with no clear seasonal variation. Apart from BJ and YD, NO₂ emissions from other regions in CEC also expand considerably.     

An anticyclonic point of view on low-level tropospheric long-range transport

Research on Arctic haze has provided an example when anticyclones may play a dominant role in carrying out low-level tropospheric long-range transport. This dominant role of anticyclones in transporting Arctic haze may be the result of the unique geographic and climatological situation existing during winter/spring in which both the huge Eurasian continent and the adjacent ice-covered Arctic Ocean tend to be regions where anticyclones form and exist over long periods of the winter and spring seasons. It is assumed that the seasonal variation of transport mechanisms provided by anticyclones is the primary cause for the seasonal variation of Arctic haze. Centers of anticyclones are the regions where air masses form and obtain their characteristics, both meteorological and chemical, due to the aerosols and gases released into the air. Transport within an air flow along the edges of quasi-stationary anticyclones will remain under stable atmospheric conditions, hence, dilution, lifting and removal of aerosols and gases will be less compared to a transport within the influence of a cyclonic pressure system. According to the concept of isentropic flow, anticyclones may dominate only low-level transport, whereas cyclones may be more important in controlling transport at upper tropospheric levels.     

Impact of biogenic terpene emissions from <Emphasis Type="Italic">Brassica napus</Emphasis> on tropospheric ozone over saxony (Germany)

INTRODUCTION: The role of biogenic emissions in tropospheric ozone production is currently under discussion and major aspects are not well understood yet. This study aims towards the estimation of the influence of biogenic emissions on tropospheric ozone concentrations over Saxony in general and of biogenic emissions from brassica napus in special. MODELLING TOOLS: The studies are performed by utilizing a coupled numerical modelling system consisting of the meteorological model METRAS and the chemistry transport model MUSCAT. For the chemical part, the Euro-RADM algorithm is used. EMISSIONS: Anthropogenic and biogenic emissions are taken into account. The anthropogenic emissions are introduced by an emission inventory. Biogenic emissions, VOC and NO, are calculated within the chemical transport model MUSCAT at each time step and in each grid cell depending on land use type and on the temperature. The emissions of hydrocarbons from forest areas as well as biogenic NO especially from agricultural grounds are considered. Also terpene emissions from brassica napus fields are estimated. SIMULATION SETUP AND METEOROLOGICAL CONDITIONS: The simulations were performed over an area with an extension of 160 x 140 km2 which covers the main parts of Saxony and neighboring areas of Brandenburg, Sachsen-Anhalt and Thuringia. Summer smog with high ozone concentrations can be expected during high pressure conditions on hot summer days. Typical meteorological conditions for such cases were introduced in an conceptual way. RESULTS: It is estimated that biogenic emissions change tropospheric ozone concentrations in a noticeable way (up to 15% to 20%) and, therefore, should not be neglected in studies about tropospheric ozone. Emissions from brassica napus do have a moderate potential to enhance tropospheric ozone concentrations, but emissions are still under consideration and, therefore, results vary to a high degree. CONCLUSIONS: Summing up, the effect of brassica napus terpene emissions on ozone concentrations is noticeable, but not too pronounced. The results give a preliminary estimate on what the effect due to brassica napus emissions could be until better parameterizations can be derived from measurements.     

Total gaseous concentrations in mercury in Seoul, Korea: Local sources compared to long-range transport from China and Japan

Total gaseous mercury (TGM) and carbon monoxide (CO) were measured every 5 min and hourly, respectively, in Seoul, Korea, from February 2005 through December 2006. The mean concentrations of TGM and CO were 3.44 ± 2.13 ng m⁻³ and 613 ± 323 ppbv, respectively. TGM and CO concentrations were highest during the winter and lowest during the summer. In total, 154 high TGM concentration events were identified: 86 were classified as long-range transport events and 68 were classified as local events. The TGM and CO concentrations were well correlated during all long-range transport events and were weakly correlated during local events. Five-day backward trajectory analysis for long-range transport events showed four potential source regions: China (79%), Japan (13%), the Yellow Sea (6%), and Russia (2%). Our results suggest that measured ΔTGM/ΔCO can be used to identify long-range transported mercury and to estimate mercury emissions from long-range transport.     

Pollution events over the East Mediterranean: Synergistic use of GOME,ground-based and sonde observations and models

The behaviour of ozone (O₃) and two important precursors, nitrogen dioxide (NO₂) and formaldehyde (HCHO), over the East Mediterranean in spring from 1996 to 2002 is studied in order to characterise the buildup of tropospheric O₃. The vertical distribution of O₃ observed over Crete during the Photochemical Activity and Solar Ultraviolet Radiation (PAUR II) campaign in May 1999 has been used for validation of satellite-derived data. Retrievals of O₃ columns from measurements of backscattered radiation by Global Ozone Monitoring Experiment (GOME) are compared with Total Ozone Mapping Spectrometer (TOMS), balloon, Systeme d’Analyse par Observation Zenithale (SAOZ) and LIDAR observations. The total O₃ vertical columns vary between 270 and 402 DU and correlate well with changes in air circulation patterns. The total observed variability in tropospheric O₃ is about 25 DU. Chemical box model calculations associate the GOME-observed NO₂ and HCHO tropospheric columns with a potential of daily photochemical enhancement in the tropospheric O₃ columns of about 0.8–1 DU over Crete and estimate the daily potential of regional photochemical buildup within upwind polluted air masses at about 2–8 DU. A Langrangian analysis attributes at most 10–20 DU of tropospheric O₃ to stratosphere–troposphere exchange (STE). The remainder is attributed to long-range transport of O₃ from industrial regions in Central Europe. From 1996 to 2002, in May no significant inter-annual variation in the tropospheric NO₂ and HCHO columns over Crete has been observed by GOME suggesting no detectable increase in regionally produced tropospheric O₃.     

Effects of elevated atmospheric CO2 and tropospheric O3 on tree branch growth and implications for hydrologic budgeting

The forest hydrologic budget may be impacted by increasing CO₂ and tropospheric O₃. Efficient means to quantify such effects are beneficial. We hypothesized that changes in the balance of canopy interception, stem flow, and through-fall in the presence of elevated CO₂ and O₃ could be discerned using image analysis of leafless branches. We compared annual stem flow to the results of a computerized analysis of all branches from the 2002, 2004, and 2006 annual growth whorls of 97 ten-year-old trees from the Aspen Free-Air CO₂ and O₃ Enrichment (Aspen FACE) experiment in Rhinelander, WI. We found significant effects of elevated CO₂ and O₃ on some branch metrics, and that the branch metrics were useful for predicting stem flow from birch, but not aspen. The results of this study should contribute to development of techniques for efficient characterization of effects on the forest hydrologic budget of increasing CO₂ and tropospheric O₃.