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Methodology for prediction and estimation of consequences of possible atmospheric releases of hazardous matter: "Kursk" submarine study

There are objects with some periods of higher than normal levels of risk of accidental atmospheric releases (nuclear, chemical, biological, etc.). Such accidents or events may occur due to natural hazards, human errors, terror acts, and during transportation of waste or various operations at high risk. A methodology for risk assessment is suggested and it includes two approaches: 1) probabilistic analysis of possible atmospheric transport patterns using long-term trajectory and dispersion modelling, and 2) forecast and evaluation of possible contamination and consequences for the environment and population using operational dispersion modelling. The first approach could be applied during the preparation stage, and the second - during the operation stage. The suggested methodology is applied on an example of the most important phases (lifting, transportation, and decommissioning) of the ``Kursk" nuclear submarine operation. It is found that the temporal variability of several probabilistic indicators (fast transport probability fields, maximum reaching distance, maximum possible impact zone, and average integral concentration of 137Cs) showed that the fall of 2001 was the most appropriate time for the beginning of the operation. These indicators allowed to identify the hypothetically impacted geographical regions and territories. In cases of atmospheric transport toward the most populated areas, the forecasts of possible consequences during phases of the high and medium potential risk levels based on a unit hypothetical release (e.g. 1 Bq) are performed. The analysis showed that the possible deposition fractions of 10-11 (Bq/m2) over the Kola Peninsula, and 10-12 - 10-13 (Bq/m2) for the remote areas of the Scandinavia and Northwest Russia could be observed. The suggested methodology may be used successfully for any potentially dangerous object involving risk of atmospheric release of hazardous materials of nuclear, chemical or biological nature.
Forecast, observation and modelling of a deep stratospheric intrusion event over Europe

A wide range of measurements was carried out in central and southeastern Europe within the framework of the EU project STACCATO (Influence of Stratosphere-Troposphere Exchange in a Changing Climate on Atmospheric Transport and Oxidation Capacity) with the principle goal to create a comprehensive data set on stratospheric air intrusions into the troposphere along a rather frequently observed pathway over central Europe from the North Sea to the Mediterranean Sea. The measurements were based on predictions by suitable quasi-operational trajectory calculations using ECMWF forecast data. A predicted deep Stratosphere to Troposphere Transport (STT) event, encountered during the STACCATO period on 20-21 June 2001, was followed by the measurements network almost from its inception. Observations provide evidence that the intrusion affected large parts of central and southeastern Europe. Especially, the ozone lidar observations on 20-21 June 2001 at Garmisch-Partenkirchen, Germany captured the evolution of two marked tongues of high ozone with the first one descending to nearly 2 km, thus providing an excellent data set for model intercomparisons and validation. In addition, for the first time to our knowledge concurrent surface measurements of the cosmogenic radionuclides 10Be and 7Be and their ratio 10Be/7Be are presented together as stratospheric tracers in a case study of a stratospheric intrusion. The ozone tracer columns calculated with the FLEXPART model were found to be in good agreement with water vapour satellite images, capturing the evolution of the observed dry streamers of stratospheric origin. Furthermore, the time-height cross section of ozone tracer simulated with FLEXPART over Garmisch-Partenkirchen captures many details of the evolution of the two observed high-ozone filaments measured with the IFU lidar, thus demonstrating the considerable progress in model simulations. Finally, the modelled ozone (operationally available since October 1999) from the ECMWF (European Centre for Medium-Range Weather Forecasts) atmospheric model is shown to be in very good agreement with the observations during this case study, which provides the first successful validation of a chemical tracer that is derived operationally from a weather forecast model. This suggests that coupling chemistry and weather forecast models may significantly improve both weather and chemical forecasts in the future.
On extreme atmospheric and marine nitrogen fluxes and chlorophyll-a levels in the Kattegat Strait

A retrospective analysis is carried out to investigate the importance of the vertical fluxes of nitrogen to the marine sea surface layer in which high chlorophyll a levels may cause blooms of harmful algae and subsequent turn over and oxygen depletion at the bottom of the sea. Typically nitrogen is the limiting factor for phytoplankton in the Kattegat Strait during summer periods (May to August) and the major nitrogen inputs come from the atmosphere and deep-water entrainment. The extreme reoccurrence values of nitrogen from atmospheric wet and dry deposition and deep-water flux entrainments are calculated by the periodic maximum method and the results are successfully compared to a map of chlorophyll return periods based on in-situ observations. The one-year return of extreme atmospheric wet deposition is around 60 mg N m-2 day-1 and 30 mg N m-2 day-1 for deep-water entrainment. Atmospheric nitrogen dry deposition is insignificant in the context of algal blooms. At longer time-scales e.g. at 10-year return, the nitrogen deep-water entrainment is larger than the extreme of atmospheric wet deposition. This indicates that the pool of nitrogen released from the sea bottom by deep-water entrainment forced by high winds greatly exceeds the atmospheric pool of nitrogen washed out by precipitation. At the frontal zone of the Kattegat Strait and Skagerrak, the nitrogen deep-water entrainment is very high and this explains the high 10-year return chlorophyll level at 8 mg m-3 in the Kattegat Strait. In the southern part, the extreme chlorophyll level is only 4 mg m-3 according to the statistics of a multi-year time-series of water samples. The chlorophyll level varies greatly in time and space as documented by a series of SeaWiFS satellite maps (OC4v4 algorithm) of chlorophyll ScanFish and buoy observations from an experimental period in the Kattegat Strait. It is recommended to sample in-situ chlorophyll observation collocated in time to the satellite overpasses of e.g. SeaWiFS and ENVISAT MERIS to ensure improved mapping of the chlorophyll levels in the Danish waters.
Partitioning of reactive nitrogen (NOy) and dependence on meteorological conditions in the lower free troposphere

Results of continuous nitrogen oxide (NO), nitrogen dioxide (NO2), peroxyacetyl nitrate (PAN) and total reactive nitrogen (NOy) measurements along with seasonal field campaigns of nitric acid (HNO3) and particulate nitrate (NO3-) measurements are presented for a two-year period at the high-alpine research station Jungfraujoch (JFJ), 3580 m asl. The NOy mixing ratio and partitioning is shown to strongly depend on meteorological conditions. Knowledge of these meteorological transport processes allows discrimination between undisturbed (i.e. clean) and disturbed (i.e. influenced by regional pollution sources) free tropospheric (FT) conditions at the JFJ. Median NOy concentrations during undisturbed FT periods ranged from 350 pptv (winter, December to February) to 581 pptv (spring, March to May). PAN was found to be the dominant NOy species during spring and summer, whereas NO2 was most abundant during autumn and winter. Particulate nitrate was found to contribute significantly to total NOy during thermally induced vertical transport. Föhn events, synoptical lifting (e.g. fronts) and thermally induced vertical transport resulted in mixing ratios up to 10 times higher at the JFJ compared to undisturbed FT conditions. Furthermore this meteorological variability of the NOy concentration and partitioning often dominated the seasonal variability. As a consequence the use of filters at the JFJ (and other mountainous sites) is crucial for the interpretation of data from such measurement sites. This study presents a further development of meteorological filters for the high-alpine site Jungfraujoch, which also could be modified and adapted to other mountainous measurement sites.
Relation between weather radar equation and first-order backscattering theory

Aim of this work is to provide a new insight into the physical basis of the meteorological-radar theory in attenuating media. Starting form the general integral form of the weather radar equation, a modified form of the classical weather radar equation at attenuating wavelength is derived. This modified radar equation includes a new parameter, called the range-bin extinction factor, taking into account the rainfall path attenuation within each range bin. It is shown that, only in the case of low-to-moderate attenuating media, the classical radar equation at attenuating wavelength can be used. These theoretical results are corroborated by using the radiative transfer theory where multiple scattering phenomena can be quantified. From a new definition of the radar reflectivity, in terms of backscattered specific intensity, a generalised radar equation is deduced. Within the assumption of first-order backscattering, the generalised radar equation is reduced to the modified radar equation, previously obtained. This analysis supports the conclusion that the description of radar observations at attenuating wavelength should include, in principle, first-order scattering effects. Numerical simulations are performed by using statistical relationships among the radar reflectivity, rain rate and specific attenuation, derived from literature. Results confirm that the effect of the range-bin extinction factor, depending on the considered frequency and range resolution, can be significant at X band for intense rain, while at Ka band and above it can become appreciable even for moderate rain. A discussion on the impact of these theoretical and numerical results is finally included.
Radiative effects of tropospheric ionisation

Despite the increasing evidence that cosmic ray variations may influence clouds and climate, there has been little discussion of the direct radiative effects of atmospheric ionisation. Laboratory experiments show that hydrated molecular cluster-ions, formed in the atmosphere by cosmic rays, absorb in the infra-red continuum at wavelengths of 9–12 μm. The tropospheric magnitude of this effect is estimated: transmittance anomalies from clear sky ion concentrations peak at ~2% at 10 km in the mid-latitudes. A simple isothermal clear sky atmospheric model suggests the integrated effect of the absorption is ~2 Wm−2. The effect appears detectable in existing surface data sets; surface micrometeorological data shows a significant anticorrelation between downwelling infra-red radiation and atmospheric cosmic ray ionisation. This is consistent with the infra-red attenuation observed in laboratory studies of cluster-ion absorption. If atmospheric ionisation from cosmic rays has universally direct radiative effects, then reinterpretation of satellite cloud data may be necessary.
Dynamics and chemistry of vortex remnants in late Arctic spring 1997 and 2000: Simulations with the Chemical Lagrangian Model of the Stratosphere (CLaMS)

High-resolution simulations of the chemical composition of the Arctic stratosphere during late spring 1997 and 2000 were performed with the Chemical Lagrangian Model of the Stratosphere (CLaMS). The simulations were performed for the entire northern hemisphere on two isentropic levels 450 K (~18 km) and 585 K (~24 km). The spatial distribution and the lifetime of the vortex remnants formed after the vortex breakup in May 1997 display different behavior above and below 20 km. Above 20 km, vortex remnants propagate southward (up to 40°N) and are "frozen in' in the summer circulation without significant mixing. Below 20 km the southward propagation of the remnants is bounded by the subtropical jet. Their lifetime is shorter by a factor of 2 than that above 20 km, owing to significant stirring below this altitude. The behavior of vortex remnants formed in March 2000 is similar but, due to an earlier vortex breakup, dominated during the first 6 weeks after the vortex breakup by westerly winds, even above 20 km. Vortex remnants formed in May 1997 are characterized by large mixing ratios of HCl indicating negligible, halogen-induced ozone loss. In contrast, mid-latitude ozone loss in late boreal spring 2000 is dominated, until mid-April, by halogen-induced ozone destruction within the vortex remnants, and subsequent transport of the ozone-depleted polar air masses (dilution) into the mid-latitudes. By varying the intensity of mixing in CLaMS, the impact of mixing on the formation of ClONO2 and ozone depletion is investigated. We find that the photochemical decomposition of HNO3 and not mixing with NOx-rich mid-latitude air is the main source of NOx within the vortex remnants in March and April 2000. Ozone depletion in the remnants is driven by ClOx photolytically formed from ClONO2. At the end of May 1997, the halogen-induced ozone deficit at 450 K poleward of 30°N amounts to ~12% with ~10% in the polar vortex and ~2% in well-isolated vortex remnants after the vortex breakup.
The roles of dynamical variability and aerosols in cirrus cloud formation

The probability of occurrence of ice crystal number densities in young cirrus clouds is examined based on airborne measurements. The observations have been carried out at midlatitudes in both hemispheres at equivalent latitudes (52-55°N/S) during the same season (local autumn in 2000). The in situ measurements considered in the present study include temperatures, vertical velocities, and total ice crystal concentrations, the latter determined with high precision and accuracy using a counterflow virtual impactor. Most young cirrus clouds typically contain high number densities (1-10 cm-3) of small (diameter <20 mm) ice crystals. This mode dominates the probability distributions and is shown to be caused by rapid cooling rates associated with updraft speeds in the range 10-100 cm s-1. A second mode containing larger crystals extends from ~1 cm-3 to low concentrations close to the detection threshold (~3 x 10-4 cm-3) and could be associated with lower updraft speeds. Results of a statistical analysis provide compelling evidence that the dynamical variability of vertical air motions on the mesoscale is the key factor determining the observed probability distributions of pristine ice crystal concentrations in cirrus. Other factors considered are changes of temperature as well as size, number, and ice nucleation thresholds of the freezing aerosol particles. The variability in vertical velocities is caused by atmospheric gravity waves leading to small-scale temperature fluctuations. Inasmuch as gravity waves are widespread, mesoscale variability in vertical velocities can be viewed as a universal feature of young cirrus clouds. Large-scale models that do not account for this subgrid-scale variability yield erroneous predictions of the variability of basic cirrus cloud properties. Climate change may bring about changes in the global distribution of updraft speeds, mean air temperatures, and aerosol properties. As shown in this work, these changes could significantly modify the probability distribution of cirrus ice crystal concentrations. This study emphasizes the key role of vertical velocities and mesoscale variability in vertical velocities in controlling cirrus properties. The results suggest that, in any effort to ascribe cause to trends of cirrus cloud properties, a careful evaluation of dynamical changes in cloud formation should be done before conclusions regarding the role of other anthropogenic factors, such as changes in aerosol composition, are made.
Formaldehyde over the eastern Mediterranean during MINOS: Comparison of airborne in-situ measurements with 3D-model results

Formaldehyde (HCHO) is an important intermediate product in the photochemical degradation of methane and non-methane volatile organic compounds. In August 2001, airborne formaldehyde measurements based on the Hantzsch reaction technique were performed during the Mediterranean INtensive Oxidant Study, MINOS. The detection limit of the instrument was 42 pptv (1s) at a time resolution of 180 s (10-90%). The overall uncertainty of the HCHO measurements was 30% at a mixing ratio of 300 pptv. In the marine boundary layer over the eastern Mediterranean Sea average HCHO concentrations were of the order of 1500 pptv, in reasonable agreement with results from a three-dimensional global chemical transport model of the lower atmosphere including non-methane volatile organic compound (NMVOC) chemistry. Above the boundary layer HCHO mixing ratios decreased with increasing altitude to a minimum level of 250 pptv at about 7 km. At higher altitudes (above 7 km) HCHO levels showed a strong dependency on the airmass origin. In airmasses from the North Atlantic/North American area HCHO levels were of the order of 300 pptv, a factor of 6 higher than values predicted by the model. Even higher HCHO levels, increasing to values of the order of 600 pptv at 11 km altitude, were observed in easterlies transporting air affected by the Indian monsoon outflow towards the Mediterranean basin. Only a small part (~30 pptv) of the large discrepancy between the model results and the measurements of HCHO in the free troposphere could be explained by a strong underestimation of the upper tropospheric acetone concentration by up to a factor of ten by the 3D-model. Therefore, the measurement-model difference in the upper troposphere remains unresolved, while the observed dependency of HCHO on airmass origin might indicate that unknown, relatively long-lived NMVOCs - or their reaction intermediates - associated with biomass burning are at least partially responsible for the observed discrepancies.
Long term measurements of submicrometer urban aerosols: statistical analysis for correlations with meteorological conditions and trace gases

Long-term measurements (over 4 years) of particle number size distributions (submicrometer particles, 3-800 nm in diameter), trace gases (NO, NO2, and O3), and meteorological parameters (global radiation, wind speed and direction, atmospheric pressure, etc.) were taken in a moderately polluted site in the city of Leipzig (Germany). The resulting complex data set was analyzed with respect to seasonal, weekly, and diurnal variation of the submicrometer aerosol. Car traffic produced a peak in the number size distribution at around 20 nm particle diameter during morning rush hour on weekdays. A second peak at 10-15 nm particle diameter occurred around noon during summer, confirmed by high correlation between concentration of particles less than 20 nm and the global radiation. This new-particle formation at noon was correlated with the amount of global radiation. A high concentration of accumulation mode particles (between 100 and 800 nm), which are associated with large particle-surface area, might prevent this formation. Such high particle concentration in the ultrafine region (particles smaller than 20 nm in diameter) was not detected in the particle mass, and thus, particle mass concentration is not suitable for determining the diurnal patterns of particles. In summer, statistical time series analysis showed a cyclic pattern of ultrafine particles with a period of one day and confirmed the correlation with global radiation. Principal component analysis (PCA) revealed a strong correlation between the particle concentration for 20-800 nm particles and the NO- and NO2-concentrations, indicating the influence of combustion processes on this broad size range, in particular during winter. In addition, PCA also revealed that particle concentration depended on meteorological conditions such as wind speed and wind direction, although the dependence differed with particle size class.