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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<sup>+</sup> from the years 1996–2001. There is no correlation between theoretical mass flux rates and changes in the Mg and Mg<sup>+</sup> 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.
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This paper reports the first record of extreme ozone measurements in Africa. As part of the AMMA program, the ozone vertical profile recorded on 20 December over Cotonou presents exceptionally high ozone concentrations with up to 295 ppb at 1 km altitude. Retroplumes from the Flexpart model show that the air masses sampled at 1 km over Cotonou on this day came from the burning area situated north-east of Cotonou and passed over Lagos, Nigeria, which is highly impacted by urban pollution. We used the Master Mechanism box model to simulate the chemical composition of the plume during its transit. <br><br> We find that neither the biomass burning emissions of ozone precursors nor additional urban emissions from Lagos are high enough to simulate more than 120–150 ppb of ozone. The only way to reach almost 300 ppb of ozone within a few hours is to feed the air mass with large amounts of reactive VOCs as those recorded in the vicinity of petrochemical area. Sensitivity tests show that 250–600 ppb of VOCs combined with 35–80 ppb of NO<sub>x</sub> allow the ozone concentrations to be higher than 250 ppb. Nigeria is the first African country with gas extraction and petrochemical industries, and petrochemical explosions frequently happen in the vicinity of Lagos. The hypothesis of a petrochemical explosion in this area is the most likely scenario which could explain the 295 ppb ozone maximum measured over Cotonou, downwind of Lagos.
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In this paper, spectra of aerosol optical thickness from the AERONET (AErosol RObotic NETwork) station at Hornsund in the southern part of Spitsbergen were employed to study the impact of air mass history on aerosol optical thickness for wavelength λ=500 nm – AOT(500) – and the Ångström exponent. Backward trajectories computed, using the NOAA HYSPLIT model, were used to trace air history. It was found that in spring, the changes in AOT values over the Hornsund station were strongly influenced by air mass trajectories 8 days or longer in duration, arriving both in the free troposphere and at an altitude of 1 km above sea level. Nevertheless, free tropospheric advection was dominant. AOT variability in summer was best explained by the local direction and speed of advection (1-day trajectories) and was dominated by the effectiveness of cleansing processes. During the ASTAR 2007 campaign, the aerosols near Hornsund displayed low AOT values ranging from 0.06 to 0.09, which is lower than the mean AOT(500) for spring seasons from 2005 to 2007 (0.110±0.007; mean ± standard deviation of mean). 9 April 2007 with AOT(500)=0.147 was exceptional. The back-trajectories belonged to clusters with low and average cluster mean AOT. Apart from the maximum AOT of 9 April 2007, the observed AOT values were close to or lower than the means for the clusters to which they belonged.
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During the ASTAR (Arctic Study of Tropospheric Aerosol and Radiation) campaign nucleation mode particles (4 to 13 nm) were quite frequently observed at altitudes below 4000 m. However, in the upper free troposphere, nucleation mode particles were only observed once, namely during the flight on 24 May 2004 (7000 m). To investigate if vertical motion were the reason for this difference that on one particular day nucleation mode particles were observed but not on the other days we employ a microphysical box model. The box model simulations were performed along air parcel trajectories calculated 6-d backwards based on European Center for Medium-Range Weather Forecasts (ECMWF) meteorological analyses using state parameters such as pressure and temperature in combination with additional parameters such as vertical stability. Box model simulations were performed for the 24 May where nucleation mode particles were observed (nucleation event) as well as for the days with measurements before and after (22 and 26 May) which are representative for no nucleation (non-nucleation event). A nucleation burst was simulated along all trajectories, however, in the majority of the simulations the nucleation rate was either too low or too high so that no nucleation mode particles were left at the time when the measurements were performed. Further, the simulation results could be divided into three cases. Thereby, we found that for case 1 the temperature was the only driving mechanism for the formation of new particles while for case 2 and 3 vertical motion have influenced the formation of new particles. The reason why nucleation mode particles were observed on 24 May, but not on the other days, can be explained by the conditions under which particle formation occurred. On 24 May the particle formation was caused by a slow updraft, while on the other two days the particle formation was caused by a fast updraft.
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Fractional release factors (FRFs) of organic trace gases are time-independent quantities that influence the calculation of Global Warming Potentials and Ozone Depletion Potentials. We present the first set of vertically resolved FRFs for 15 long-lived halocarbons in the tropical stratosphere up to 34 km altitude. They were calculated from measurements on air samples collected on board balloons and a high altitude aircraft. We compare the derived dependencies of FRFs on the mean stratospheric transit times (the so-called mean ages of air) with similarly derived FRFs originating from measurements at higher latitudes and find significant differences. Moreover a comparison with averaged FRFs currently used by the World Meteorological Organisation revealed the limitations of these measures due to their observed vertical and latitudinal variability. The presented data set could be used to improve future ozone level and climate projections.
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In anthropogenically influenced atmospheres, sulphur dioxide (SO<sub>2</sub>) is the main precursor of gaseous sulphuric acid (H<sub>2</sub>SO<sub>4</sub>), which in turn is a main precursor for atmospheric particle nucleation. As a result of socio-economic changes, East Germany has seen a dramatic decrease in anthropogenic SO<sub>2</sub> emissions between 1989 and present, as documented by routine air quality measurements in many locations. We have attempted to evaluate the influence of changing SO<sub>2</sub> concentrations on the frequency and intensity of new particle formation (NPF) using two different data sets (1996–1997; 2003–2006) of experimental particle number size distributions (diameter range 3–750 nm) from the atmospheric research station Melpitz near Leipzig, Germany. Between the two periods SO<sub>2</sub> concentrations decreased by 65% on average, while the frequency of NPF events dropped by 45%. Meanwhile, the average formation rate of 3 nm particles decreased by 68% on average. The trends were statistically significant and therefore suggest a connection between the availability of anthropogenic SO<sub>2</sub> and freshly formed new particles. In contrast to the decrease in new particle formation, we found an increase in the mean growth rate of freshly nucleated particles (+22%), suggesting that particle nucleation and subsequent growth into larger sizes are delineated with respect to their precursor species. Using three basic parameters, the condensation sink for H<sub>2</sub>SO<sub>4</sub>, the SO<sub>2</sub> concentration, and the global radiation intensity, we were able to define the characteristic range of atmospheric conditions under which particle formation events take place at the Melpitz site. While the decrease in the concentrations and formation rates of the new particles was rather evident, no similar decrease was found with respect to the generation of cloud condensation nuclei (CCN; particle diameter >100 nm) as a result of atmospheric nucleation events. On the contrary, the production of CCN following nucleation events appears to have increased by tens of percents. Our aerosol dynamics model simulations suggest that such an increase can be caused by the increased particle growth rate.
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Recent results from diverse air, ground, and laboratory studies using both radiometric and in situ techniques show that the fractions of black carbon, organic matter, and mineral dust in atmospheric aerosols determine the wavelength dependence of absorption (often expressed as Absorption Angstrom Exponent, or AAE). Taken together, these results hold promise of improving information on aerosol composition from remote measurements. The main purpose of this paper is to show that AAE values for an Aerosol Robotic Network (AERONET) set of retrievals from Sun-sky measurements describing full aerosol vertical columns are also strongly correlated with aerosol composition or type. In particular, we find AAE values near 1 (the theoretical value for black carbon) for AERONET-measured aerosol columns dominated by urban-industrial aerosol, larger AAE values for biomass burning aerosols, and the largest AAE values for Sahara dust aerosols. These AERONET results are consistent with results from other, very different, techniques, including solar flux-aerosol optical depth (AOD) analyses and airborne in situ analyses examined in this paper, as well as many other previous results. Ambiguities in aerosol composition or mixtures thereof, resulting from intermediate AAE values, can be reduced via cluster analyses that supplement AAE with other variables, for example Extinction Angstrom Exponent (EAE), which is an indicator of particle size. Together with previous results, these results strengthen prospects for determining aerosol composition from space, for example using the Glory Aerosol Polarimetry Sensor (APS), which seeks to provide retrievals of multiwavelength single-scattering albedo (SSA) and aerosol optical depth (and therefore aerosol absorption optical depth (AAOD) and AAE), as well as shape and other aerosol properties. Multidimensional cluster analyses promise additional information content, for example by using the Ozone Monitoring Instrument (OMI) to add AAOD in the near ultraviolet and CALIPSO aerosol layer heights to reduce height-absorption ambiguity.
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Due to increasing atmospheric concentration of greenhouse gases and changing stratospheric ozone concentration, both of anthropogenic origin, various quantities in the middle atmosphere reveal long-term changes and trends. Lastovicka and Krizan (2006) indicated possibility of change of trends in the dynamics in the northern midlatitude middle atmosphere as a whole in the 1990s. To search for such change of trends we use data on winds in the mesopause region, on total columnar ozone, on ozone laminae, on winds in the middle and lower stratosphere, and on peak electron density in the E region of the ionosphere. One group of quantities, the mesopause region wind-like trends, changes their trends around 1990, the other one, the total ozone-like trends, in the mid-1990s. Altogether they create a skeleton of scenario of the change of the middle atmosphere dynamics trends in the 1990s. Drivers of these changes appear to be different for the first group and for the second group. Tropospheric processes seem to play a role in the changes of trends in middle atmospheric dynamics.
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We evaluate the effect of varying the temporal resolution of the input climate data on isoprene emission estimates generated by the community emissions model MEGAN (Model of Emissions of Gases and Aerosols from Nature). The estimated total global annual emissions of isoprene is reduced from 766 Tg y<sup>−1</sup> when using hourly input data to 746 Tg y<sup>−1</sup> (a reduction of 3%) for daily average input data and 711 Tg y<sup>−1</sup> (down 7%) for monthly average input data. The impact on a local scale can be more significant with reductions of up to 55% at some locations when using monthly average data compared with using hourly data. If the daily and monthly average temperature data are used without the imposition of a diurnal cycle the global emissions estimates fall by 27–32%, and local annual emissions by up to 77%. A similar pattern emerges if hourly isoprene fluxes are considered. In order to better simulate and predict isoprene emission rates using MEGAN, we show it is necessary to use temperature and radiation data resolved to one hour. Given the importance of land-atmosphere interactions in the Earth system and the low computational cost of the MEGAN algorithms, we recommend that chemistry-climate models and the new generation of Earth system models input biogenic emissions at the highest temporal resolution possible.
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This paper presents the first global set of observations of CO<sub>2</sub> in the mesosphere and lower thermosphere (MLT) obtained by the ACE-FTS instrument on SCISAT-I, a small Canadian satellite launched in 2003. The observations use the solar occultation technique and document the fall-off in the mixing ratio of CO<sub>2</sub> in the MLT region. The beginning of the fall-off of the CO<sub>2</sub>, or "knee" occurs at about 78 km and lies higher than in the CRISTA-1 measurements (~70 km) but lower than in the SABER 1.06 (~80 km) and much lower than in rocket measurements. We also present the measurements of CO obtained concurrently which provide important constraints for analysis. We have compared the ACE measurements with simulations of the CO<sub>2</sub> and CO distributions in the vertically extended version of the Canadian Middle Atmosphere Model (CMAM). Applying standard chemistry we find that we cannot get agreement between the model and ACE CO<sub>2</sub> observations although the CO observations are adequately reproduced. There appears to be about a 10 km offset compared to the observed ACE CO<sub>2</sub>, with the model "knee" occurring too high. In analyzing the disagreement, we have investigated the variation of several parameters of interest (photolysis rates, formation rate for CO<sub>2</sub>, and the impact of uncertainty in turbulent eddy diffusion) in order to explore parameter space for this problem. Our conclusions are that there must be a loss process for CO<sub>2</sub>, about 2–4~times faster than photolysis that will sequester the carbon in some form other than CO and we have speculated on the role of meteoritic dust as a possible candidate. In addition, from this study we have highlighted a possible important role for unresolved vertical eddy diffusion in 3-D models in determining the distribution of candidate species in the mesosphere which requires further study.
