MOCRA: a Monte Carlo code for the simulation of radiative transfer in the atmosphere.

This paper describes the radiative transfer model (RTM) MOCRA (MOnte Carlo Radiance Analysis), developed in the frame of DOAS (Differential Optical Absorption Spectroscopy) to correctly interpret remote sensing measurements of trace gas amounts in the atmosphere through the calculation of the Air Mass Factor. Besides the DOAS-related quantities, the MOCRA code yields: 1- the atmospheric transmittance in the vertical and sun directions, 2- the direct and global irradiance, 3- the single- and multiple- scattered radiance for a detector with assigned position, line of sight and field of view. Sample calculations of the main radiometric quantities calculated with MOCRA are presented and compared with the output of another RTM (MODTRAN4). A further comparison is presented between the NO2 slant column densities (SCDs) measured with DOAS at Evora (Portugal) and the ones simulated with MOCRA. Both comparisons (MOCRA-MODTRAN4 and MOCRA-observations) gave more than satisfactory results, and overall make MOCRA a versatile tool for atmospheric radiative transfer simulations and interpretation of remote sensing measurements

Morphology of the tropopause layer and lower stratosphere above a tropical cyclone : a case study on cyclone Davina (1999)

During the APE-THESEO mission in the Indian Ocean the Myasishchev Design Bureau stratospheric research aircraft M55 Geophysica performed a flight over and within the inner core region of tropical cyclone Davina. Measurements of total water, water vapour, temperature, aerosol backscattering, ozone and tracers were made and are discussed here in comparison with the averages of those quantities acquired during the campaign time frame. Temperature anomalies in the tropical tropopause layer (TTL), warmer than average in the lower part and colder than average in the upper TTL were observed. Ozone was strongly reduced compared to its average value, and thick cirrus decks were present up to the cold point, sometimes topped by a layer of very dry air. Evidence for meridional transport of trace gases in the stratosphere above the cyclone was observed and perturbed water distribution in the TTL was documented. The paper discuss possible processes of dehydration induced by the cirrus forming above the cyclone, and change in the chemical tracer and water distribution in the lower stratosphere 400–430 K due to meridional transport from the mid-latitudes and link with Davina. Moreover it compares the data prior and after the cyclone passage to discuss its actual impact on the atmospheric chemistry and thermodynamics

Recent results from the Arctic Radiation and Turbulence Interaction STudy (ARTIST) project

Ground-based measurements were conducted at Ny-˚Alesund in the Svalbard Islands in the framework of the research project ARTIST (Arctic Radiation and Turbulence Interaction STudy) funded by the European Communities. Key objectivesof the campaign were: 1) provide all participantswith ground reference data as input to models describing the development of the atmospheric boundary level, 2) compute the surface roughness length in order to characterise the surface of the site, 3) parameterise the surface energy exchanges, calculating the surface radiation flux, the sensible and latent heat fluxes, and 4) obtain the surface energy balance during both clear and cloudy sky conditions. The cloud radiative forcing has been also estimated. Final results of the analysis of the data set are presented

Diagnostics of the Tropical Tropopause Layer from in-situ observations and CCM data

A suite of diagnostics is applied to in-situ aircraft measurements and one Chemistry-Climate Model (CCM) data to characterize the vertical structure of the Tropical Tropopause Layer (TTL). The diagnostics are based on vertical tracer profiles and relative vertical tracer gradients, using tropopause-referenced coordinates, and tracer-tracer relationships in the tropical Upper Troposphere/Lower Stratosphere (UT/LS). <br><br> Observations were obtained during four tropical campaigns performed from 1999 to 2006 with the research aircraft Geophysica and have been compared to the output of the ECHAM5/MESSy CCM. The model vertical resolution in the TTL (~500 m) allows for appropriate comparison with high-resolution aircraft observations and the diagnostics used highlight common TTL features between the model and the observational data. <br><br> The analysis of the vertical profiles of water vapour, ozone, and nitrous oxide, in both the observations and the model, shows that concentration mixing ratios exhibit a strong gradient change across the tropical tropopause, due to the role of this latter as a transport barrier and that transition between the tropospheric and stratospheric regimes occurs within a finite layer. The use of relative vertical ozone and carbon monoxide gradients, in addition to the vertical profiles, helps to highlight the region where this transition occurs and allows to give an estimate of its thickness. The analysis of the CO-O<sub>3</sub> and H<sub>2</sub>O-O<sub>3</sub> scatter plots and of the Probability Distribution Function (PDF) of the H<sub>2</sub>O-O<sub>3</sub> pair completes this picture as it allows to better distinguish tropospheric and stratospheric regimes that can be identified by their different chemical composition. <br><br> The joint analysis and comparison of observed and modelled data allows to state that the model can represent the background TTL structure and its seasonal variability rather accurately. The model estimate of the thickness of the interface region between tropospheric and stratospheric regimes agrees well with average values inferred from observations. On the other hand, the measurements can be influenced by regional scale variability, local transport processes as well as deep convection, that can not be captured by the model

Impact of deep convection in the tropical tropopause layer in West Africa: in-situ observations and mesoscale modelling

We present the analysis of the impact of convection on the composition of the tropical tropopause layer region (TTL) in West-Africa during the AMMA-SCOUT campaign. Geophysica M55 aircraft observations of water vapor, ozone, aerosol and CO<sub>2</sub> during August 2006 show perturbed values at altitudes ranging from 14 km to 17 km (above the main convective outflow) and satellite data indicates that air detrainment is likely to have originated from convective cloud east of the flights. Simulations of the BOLAM mesoscale model, nudged with infrared radiance temperatures, are used to estimate the convective impact in the upper troposphere and to assess the fraction of air processed by convection. The analysis shows that BOLAM correctly reproduces the location and the vertical structure of convective outflow. Model-aided analysis indicates that convection can influence the composition of the upper troposphere above the level of main outflow for an event of deep convection close to the observation site. Model analysis also shows that deep convection occurring in the entire Sahelian transect (up to 2000 km E of the measurement area) has a non negligible role in determining TTL composition

Vertical profile of peroxyacetyl nitrate (PAN) from MIPAS-STR measurements over Brazil in February 2005 and its contribution to tropical UT NOy partitioning

We report on the retrieval of PAN (CH₃C(O)OONO₂) in the upper tropical troposphere from limb measurements by the remote-sensor MIPAS-STR on board the Russian high altitude research aircraft M55-Geophysica. The measurements were performed close to Araçatuba, Brazil, on 17 February 2005. The retrieval was made in the spectral range 775–820 cm^&minus;1 where PAN exhibits its strongest feature but also more than 10 species interfere. Especially trace gases such as CH₃CCl₃, CFC-113, CFC-11, and CFC-22, emitting also in spectrally broad not-resolved branches, make the processing of PAN prone to errors. Therefore, the selection of appropriate spectral windows, the separate retrieval of several interfering species and the careful handling of the water vapour profile are part of the study presented. <br><br> The retrieved profile of PAN has a maximum of about 0.14 ppbv at 10 km altitude, slightly larger than the lowest reported values (&lt;0.1 ppbv) and much lower than the highest reported in the literature (0.65 ppbv). Besides the NO_y constituents measured by MIPAS-STR (HNO₃, ClONO₂, HO₂NO₂, PAN), the in situ instruments aboard the Geophysica provide simultaneous measurements of NO, NO₂, and the sum NO_y. Comparing the sum of in-situ and remotely derived NO+NO₂+HNO₃+ClONO₂+HO₂NO₂+PAN with total NO_y a deficit of 30–40% (0.2–0.3 ppbv) in the troposphere remains unexplained whereas the values fit well in the stratosphere

Perspectives of 2D and 3D mapping of atmospheric pollutants over urban areas by means of airborne DOAS spectrometers

tants, offering numerous advantages over conventional networks of in situ analysers. We propose some innovative solutions in the field of DOAS (Differential Optical Absorption Spectroscopy) remote systems, utilizing diffuse solar light as the radiation source. We examine the numerous potentialities of minor gas slant column calculations, applying the «off-axis» methodology for collecting the diffuse solar radiation. One of these particular approaches, using measurements along horizontal paths, has already been tested with the spectrometer installed on board the Geophysica aircraft during stratospheric flights up to altitudes of 20 km. The theoretical basis of these new measurement techniques using DOAS remote sensing systems are delineated to assess whether low altitude flights can provide 2D and 3D pollution tomography over metropolitan areas. The 2D or 3D trace gas total column mapping could be used to investigate: i) transport and dispersion phenomena of air pollution, ii) photochemical process rates, iii) gas plume tomography, iv) minor gas vertical profiles into the Planetary Boundary Layer and v) minor gas flux divergence over a large area

In situ measurements of tropical cloud properties in the West African Monsoon: upper tropospheric ice clouds, Mesoscale Convective System outflow, and subvisual cirrus

In situ measurements of ice crystal size distributions in tropical upper troposphere/lower stratosphere (UT/LS) clouds were performed during the SCOUT-AMMA campaign over West Africa in August 2006. The cloud properties were measured with a Forward Scattering Spectrometer Probe (FSSP-100) and a Cloud Imaging Probe (CIP) operated aboard the Russian high altitude research aircraft M-55 Geophysica with the mission base in Ouagadougou, Burkina Faso. A total of 117 ice particle size distributions were obtained from the measurements in the vicinity of Mesoscale Convective Systems (MCS). Two to four modal lognormal size distributions were fitted to the average size distributions for different potential temperature bins. The measurements showed proportionately more large ice particles compared to former measurements above maritime regions. With the help of trace gas measurements of NO, NOy, CO2, CO, and O3 and satellite images, clouds in young and aged MCS outflow were identified. These events were observed at altitudes of 11.0 km to 14.2 km corresponding to potential temperature levels of 346 K to 356 K. In a young outflow from a developing MCS ice crystal number concentrations of up to (8.3 ± 1.6) cm−3 and rimed ice particles with maximum dimensions exceeding 1.5 mm were found. A maximum ice water content of 0.05 g m−3 was observed and an effective radius of about 90 μm. In contrast the aged outflow events were more diluted and showed a maximum number concentration of 0.03 cm−3, an ice water content of 2.3 × 10−4 g m−3, an effective radius of about 18 μm, while the largest particles had a maximum dimension of 61 μm. Close to the tropopause subvisual cirrus were encountered four times at altitudes of 15 km to 16.4 km. The mean ice particle number concentration of these encounters was 0.01 cm−3 with maximum particle sizes of 130 μm, and the mean ice water content was about 1.4 × 10−4 g m−3. All known in situ measurements of subvisual tropopause cirrus are compared and an exponential fit on the size distributions is established for modelling purposes. A comparison of aerosol to ice crystal number concentrations, in order to obtain an estimate on how many ice particles may result from activation of the present aerosol, yielded low ratios for the subvisual cirrus cases of roughly one cloud particle per 30 000 aerosol particles, while for the MCS outflow cases this resulted in a high ratio of one cloud particle per 300 aerosol particles

Contribution of mixing to the upward transport across the TTL

International audienceDuring the second part of the TROCCINOX campaign that took place in Brazil in early 2005, chemical species were measured on-board of the high altitude research aircraft Geophysica (ozone, water vapor, NO, NOy, CH4 and CO) in the altitude range up to 20 km (or up to 450 K potential temperature), i.e. spanning the TTL region roughly extending between 350 and 420 K. Analysis of transport across TTL is performed using a new version of the Chemical Lagrangian Model of the Stratosphere (CLaMS). In this new version, the stratospheric model has been extended to the earth surface. Above the tropopause, the isentropic and cross-isentropic advection in CLaMS is driven by ECMWF winds and heating/cooling rates derived from a radiation calculation. Below the tropopause the model smoothly transforms from the isentropic to hybrid-pressure coordinate and, in this way, takes into account the effect of large-scale convective transport as implemented in the ECMWF vertical wind. As with other CLaMS simulations, the irreversible transport, i.e. mixing, is controlled by the local horizontal strain and vertical shear rates. Stratospheric and tropospheric signatures in the TTL can be seen both in the observation and in the model. The composition of air above ?350 K is mainly controlled by mixing on a time scale of weeks or even months. Based on CLaMS transport studies where mixing can be completely switched off, we deduce that vertical mixing, mainly driven by the vertical shear in the outflow regions of the large-scale convection and in the vicinity of the subtropical jets, is necessary to understand the upward transport of the tropospheric air from the main convective outflow around 350 K up to the tropical tropopause around 380 K. This mechanism is most effective if the outflow of the mesoscale convective systems interacts with the subtropical jets