Items

Advanced search

Quantification of the impact in mid-latitudes of chemical ozone depletion in the 1999/2000 Arctic polar vortex prior to the vortex breakup

For the winter 1999/2000 transport of air masses out of the vortex to mid-latitudes and ozone destruction inside and outside the northern polar vortex is studied to quantify the impact of earlier winter (before March) polar ozone destruction on mid-latitude ozone. Nearly 112 000 trajectories are started on 1 December 1999 on 6 different potential temperature levels between 500–600 K and for a subset of these trajectories photo-chemical box-model calculations are performed. We linked a decline of −0.9% of mid-latitude ozone in this layer occurring in January and February 2000 to ozone destruction inside the vortex and successive transport of these air masses to mid-latitudes. Further, the impact of denitrification, PSC-occurrence and anthropogenic chlorine loading on future stratospheric ozone is determined by applying various scenarios. Lower stratospheric temperatures and denitrification were found to play the most important role in the future evolution of polar ozone depletion.
Validation of the calibration of a laser-induced fluorescence instrument for the measurement of OH radicals in the atmosphere

An assessment of the accuracy of OH concentrations measured in a smog chamber by a calibrated laser-induced fluorescence (LIF) instrument has been made, in the course of 9 experiments performed to study the photo-oxidation of benzene, toluene, 1,3,5-trimethylbenzene, para-xylene, ortho-cresol and ethene at the European Photoreactor facility (EUPHORE). The LIF system was calibrated via the water photolysis / ozone actinometry approach. OH concentrations were inferred from the instantaneous rate of removal of each hydrocarbon species (measured by FTIR or HPLC) via the appropriate rate coefficient for their reaction with OH, and compared with those obtained from the LIF system. Good agreement between the two approaches was found for all species with the exception of 1,3,5-trimethylbenzene, for which OH concentrations inferred from hydrocarbon removal were a factor of 3 lower than those measured by the LIF system. From the remaining 8 experiments, an overall value of 1.15±0.13 (±1σ) was obtained for [OH]LIF / [OH]Hydrocarbon Decay, compared with the estimated uncertainty in the accuracy of the water photolysis / ozone actinometry OH calibration technique of 26% (1σ).
Commentary on "Improving the seasonal cycle and interannual variations of biomass burning aerosol sources" by Generoso et al.

In a recent published paper, Generoso et al. (2003) describe a method for improving the spatial and temporal distribution of pyrogenic aerosol emission inventories. In the course of their analysis, the authors note several significant discrepancies in the seasonality of burning as observed by the Visible and Infrared Scanner (VIRS) and four other biomass burning data sets derived from satellite observations. In this commentary we explain the source of these discrepancies and clarify the origin of the VIRS observations that were used by Generoso et al.
Model study of multiphase DMS oxidation with a focus on halogens

We studied the oxidation of dimethylsulfide (DMS) in the marine boundary layer (MBL) with a one-dimensional numerical model and focused on the influence of halogens. Our model runs show that there is still significant uncertainty about the end products of the DMS addition pathway, which is especially caused by uncertainty in the product yield of the reaction of the intermediate product methyl sulfinic acid (MSIA) with OH. BrO strongly increases the importance of the addition branch in the oxidation of DMS even when present at mixing ratios smaller than 0.5pmol mol-1. The inclusion of halogen chemistry leads to higher DMS oxidation rates and smaller DMS to SO2 conversion efficiencies. The DMS to SO2 conversion efficiency is also drastically reduced under cloudy conditions. In cloud-free model runs between 5 and 15% of the oxidized DMS reacts further to particulate sulfur, in cloudy runs this fraction is almost 100%. Sulfate production by HOClaq and HOBraq is important in cloud droplets even for small Br- deficits and related small gas phase halogen concentrations. In general, more particulate sulfur is formed when halogen chemistry is included. A possible enrichment of HCO3- in fresh sea salt aerosol would increase pH values enough to make the reaction of S(IV)* (=SO2,aq+HSO3-+SO32-) with O3 dominant for sulfate production. It leads to a shift from methyl sulfonic acid (MSA) to non-sea salt sulfate (nss-SO42-) production but increases the total nss-SO42- only somewhat because almost all available sulfur is already oxidized to particulate sulfur in the base scenario. We discuss how realistic this is for the MBL. We found the reaction MSAaq+OH to contribute about 10% to the production of nss-SO42- in clouds. It is unimportant for cloud-free model runs. Overall we find that the presence of halogens leads to processes that decrease the albedo of stratiform clouds in the MBL.
Effect of organic compounds on nanoparticle formation in diluted diesel exhaust

The nucleation of nanoparticles in the exhaust of a modern light-duty diesel vehicle was investigated on a chassis dynamometer. This laboratory study is focused on the influence of volatile organic compounds (VOCs) on nucleation of volatile nanoparticles. Different organic compounds were added to the dilution air of the particle sampling under different sampling conditions. Sample temperature and relative sample humidity were varied in a wide range. The number size distribution of the particles was measured with a scanning mobility particle sizer (SMPS) and showed significant differences in response to the added organic compounds. While the nucleation mode particles showed a large variation in concentration, the accumulation mode particles remained unchanged for all compounds. Depending on the functional group, organic compounds were capable of initiating and increasing (alcohols and toluene) or decreasing (acetone, aniline, and methyl tert-butyl ether (MTBE)) nucleation mode particles. Short volatile aliphatic hydrocarbons (hexane and cyclohexane) turned out to be without effect on nucleation of nanoparticles. Possible reasons for the differences are discussed.
Radiant measurement accuracy of micrometeors detected by the Arecibo 430 MHz Dual-Beam Radar

Precise knowledge of the angle between the meteor vector velocity and the radar beam axis is one of the largest source of errors in the Arecibo Observatory (AO) micrometeor observations. In this paper we study ~250 high signal-to-noise ratio (SNR) meteor head-echoes obtained using the dual-beam 430 MHz AO Radar in Puerto Rico, in order to reveal the distribution of this angle. All of these meteors have been detected first by the radar first side lobe, then by the main beam and finally seen in the side lobe again. Using geometrical arguments to calculate the meteor velocity in the plane perpendicular to the beam axis, we find that most of the meteors are travelling within ~15° with respect to the beam axis, in excellent agreement with previous estimates. These results suggest that meteoroids entering the atmosphere at greater angles may deposit their meteoric material at higher altitudes explaining at some level the missing mass inconsistency raised by the comparisson of meteor fluxes derived from satellite and traditional meteor radar observations. They also may be the source of the observed high altitude ions and metalic layers observed by radars and lidars respectively.
On the distribution of relative humidity in cirrus clouds

We have analysed relative humidity statistics from measurements in cirrus clouds taken unintentionally during the Measurement of OZone by Airbus In-service airCraft project (MOZAIC). The shapes of the in-cloud humidity distributions change from nearly symmetric in relatively warm cirrus (warmer than −40°C) to considerably positively skew (i.e. towards high humidities) in colder clouds. These results are in agreement to findings obtained recently from the INterhemispheric differences in Cirrus properties from Anthropogenic emissions (INCA) campaign (Ovarlez et al., 2002). We interprete the temperature dependence of the shapes of the humidity distributions as an effect of the length of time a cirrus cloud needs from formation to a mature equilibrium stage, where the humidity is close to saturation. The duration of this transitional period increases with decreasing temperature. Hence cold cirrus clouds are more often met in the transitional stage than warm clouds.
A time-resolved model of the mesospheric Na layer: constraints on the meteor input function

A time-resolved model of the Na layer in the mesosphere/lower thermosphere region is described, where the continuity equations for the major sodium species Na, Na+ and NaHCO3 are solved explicity, and the other short-lived species are treated in steady-state. It is shown that the diurnal variation of the Na layer can only be modelled satisfactorily if sodium species are permanently removed below about 85 km, both through the dimerization of NaHCO3 and the uptake of sodium species on meteoric smoke particles that are assumed to have formed from the recondensation of vaporized meteoroids. When the sensitivity of the Na layer to the meteoroid input function is considered, an inconsistent picture emerges. The ratio of the column abundance of Na+ to Na is shown to increase strongly with the average meteoroid velocity, because the Na is injected at higher altitudes. Comparison with a limited set of Na+ measurements indicates that the average meteoroid velocity is probably less than about 25 km s-1, in agreement with velocity estimates from conventional meteor radars, and considerably slower than recent observations made by wide aperture incoherent scatter radars. The Na column abundance is shown to be very sensitive to the meteoroid mass input rate, and to the rate of vertical transport by eddy diffusion. Although the magnitude of the eddy diffusion coefficient in the 80–90 km region is uncertain, there is a consensus between recent models using parameterisations of gravity wave momentum deposition that the average value is less than 3×105 cm2 s-1. This requires that the global meteoric mass input rate is less than about 20 td-1, which is closest to estimates from incoherent scatter radar observations. Finally, the diurnal variation in the meteoroid input rate only slight perturbs the Na layer, because the residence time of Na in the layer is several days, and diurnal effects are effectively averaged out.
The EISCAT meteor-head method – a review and recent observations

Since the very first meteor observations at EISCAT in December 1990, the experimental method has improved significantly. This is due to a better understanding of the phenomenon and a recent major upgrade of the EISCAT signal processing and data storage capabilities. Now the simultaneous spatial-time resolution is under 100 m-ms class. To illuminate the meteor target for as long as possible and simultaneously get as good altitude resolution as possible, various coding techniques have been used, such as Barker codes and random codes with extremely low side lobe effects. This paper presents some background and the current view of the meteor head echo process at EISCAT as well as the observations which support this view, such as altitude distributions, dual-frequency target sizes and vector velocities. It also presents some preliminary results from recent very high resolution tristatic observations.
Comment on “Improving the seasonal cycle and interannual variations of biomass burning aerosol sources" by Generoso et al.

Generoso et al. (2003) suggest a method for improving current inventories of aerosol emission from biomass burning based on the Along Track Scanning Radiometer (ATSR) nighttime hot spot product. In order to show the validity and representative of the nighttime burning product for such applications, Genoroso et al. (2003) compared the ATSR nighttime products to the daily fire products from TRMM, AVHRR etc. in nine selected regions. Their analyses demonstrate that in most cases, the nighttime products show a seasonal cycle that is consistent with the daily observations. However, they noticed significant discrepancies in biomass seasonality between ATSR nighttime product and TRMM daily product in Sahel region. In a commentary paper, Giglio and Kendall (2003) clarify that the origin of TRMM fire data used in Generoso et al. (2003) is from TRMM Science Data and Information System (Ji and Stocker, 2002). We thank Giglio and Kendall for such clarifications that provide an opportunity for us to clarify several issues on the applications of TSDIS fire data.