ALBERT

Description: The winter 2009/2010 was characterized by a strong Arctic vortex with extremely cold mid-winter temperatures in the lower stratosphere associated with an intense activation of reactive chlorine compounds (ClOx) from reservoir species. Stratospheric limb emission spectra were recorded during a flight of the balloon version of the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS-B) from Kiruna (Sweden) on 24 January 2010 inside the Arctic vortex. Several fast limb sequences of spectra (in time steps of about 10 min) were measured from nighttime photochemical equilibrium to local noon allowing the retrieval of chlorine- and nitrogen-containing species which change rapidly their concentration around the terminator between night and day. Mixing ratios of species like ClO, NO2, and N2O5 show significant changes around sunrise, which are temporally delayed due to polar stratospheric clouds reducing the direct radiative flux from the sun. ClO variations were derived for the first time from MIPAS-B spectra. Daytime ClO values of up to 1.6 ppbv are visible in a broad chlorine activated layer below 26 km correlated with low values (below 0.1 ppbv) of the chlorine reservoir species ClONO2. Observations are compared and discussed with calculations performed with the 3-dimensional Chemistry Climate Model EMAC (ECHAM5/MESSy Atmospheric Chemistry). Mixing ratios of the species ClO, NO2, and N2O5 are well reproduced by the model during night and noon. However, the onset of ClO production and NO2 loss around the terminator in the model is not consistent with the measurements. The MIPAS-B observations along with Tropospheric Ultraviolet-Visible (TUV) radiation model calculations suggest that polar stratospheric clouds lead to a delayed start followed by a faster increase of the photodissoziation of ClOOCl and NO2 near the morning terminator since stratospheric clouds alter the direct and the diffuse flux of solar radiation. These effects are not considered in the EMAC model simulations which assume a cloudless atmosphere.

Description: The Gimballed Limb Observer for Radiance Imaging of the Atmosphere (GLORIA), a Fourier transform spectrometer based limb spectral imager, operates on high-altitude research aircraft to study the transit region between the troposphere and the stratosphere. It is one of the most sophisticated systems to be flown on research aircraft in Europe, requiring constant monitoring and human intervention in addition to an automation system. To ensure proper functionality and interoperability on multiple platforms, a flexible control and communication system was laid out. The architectures of the communication system as well as the protocols used are reviewed. The integration of this architecture in the automation process as well as the scientific campaign flight application context are discussed.

Description: The international research project RECONCILE has addressed central questions regarding polar ozone depletion, with the objective to quantify some of the most relevant yet still uncertain physical and chemical processes and thereby improve prognostic modelling capabilities to realistically predict the response of the ozone layer to climate change. This overview paper outlines the scope and the general approach of RECONCILE, and it provides a summary of observations and modelling in 2010 and 2011 that have generated an in many respects unprecedented dataset to study processes in the Arctic winter stratosphere. Principally, it summarises important outcomes of RECONCILE including (i) better constraints and enhanced consistency on the set of parameters governing catalytic ozone destruction cycles, (ii) a better understanding of the role of cold binary aerosols in heterogeneous chlorine activation, (iii) an improved scheme of polar stratospheric cloud (PSC) processes that includes heterogeneous nucleation of nitric acid trihydrate (NAT) and ice on non-volatile background aerosol leading to better model parameterisations with respect to denitrification, and (iv) long transient simulations with a chemistry-climate model (CCM) updated based on the results of RECONCILE that better reproduce past ozone trends in Antarctica and are deemed to produce more reliable predictions of future ozone trends. The process studies and the global simulations conducted in RECONCILE show that in the Arctic, ozone depletion uncertainties in the chemical and microphysical processes are now clearly smaller than the sensitivity to dynamic variability.

Description: Significant reductions in stratospheric ozone occur inside the polar vortices each spring when chlorine radicals produced by heterogeneous reactions on cold particle surfaces in winter destroy ozone mainly in two catalytic cycles, the ClO dimer cycle and the ClO/BrO cycle. Chlorofluorocarbons (CFCs), which are responsible for most of the chlorine currently present in the stratosphere, have been banned by the Montreal Protocol and its amendments, and the ozone layer is predicted to recover to 1980 levels within the next few decades. During the same period, however, climate change is expected to alter the temperature, circulation patterns and chemical composition in the stratosphere, and possible geo-engineering ventures to mitigate climate change may lead to additional changes. To realistically predict the response of the ozone layer to such influences requires the correct representation of all relevant processes. The European project RECONCILE has comprehensively addressed remaining questions in the context of polar ozone depletion, with the objective to quantify the rates of some of the most relevant, yet still uncertain physical and chemical processes. To this end RECONCILE used a broad approach of laboratory experiments, two field missions in the Arctic winter 2009/10 employing the high altitude research aircraft M55-Geophysica and an extensive match ozone sonde campaign, as well as microphysical and chemical transport modelling and data assimilation. Some of the main outcomes of RECONCILE are as follows: (1) vortex meteorology: the 2009/10 Arctic winter was unusually cold at stratospheric levels during the six-week period from mid-December 2009 until the end of January 2010, with reduced transport and mixing across the polar vortex edge; polar vortex stability and how it is influenced by dynamic processes in the troposphere has led to unprecedented, synoptic-scale stratospheric regions with temperatures below the frost point; in these regions stratospheric ice clouds have been observed, extending over 〉106km2 during more than 3 weeks. (2) Particle microphysics: heterogeneous nucleation of nitric acid trihydrate (NAT) particles in the absence of ice has been unambiguously demonstrated; conversely, the synoptic scale ice clouds also appear to nucleate heterogeneously; a variety of possible heterogeneous nuclei has been characterised by chemical analysis of the non-volatile fraction of the background aerosol; substantial formation of solid particles and denitrification via their sedimentation has been observed and model parameterizations have been improved. (3) Chemistry: strong evidence has been found for significant chlorine activation not only on polar stratospheric clouds (PSCs) but also on cold binary aerosol; laboratory experiments and field data on the ClOOCl photolysis rate and other kinetic parameters have been shown to be consistent with an adequate degree of certainty; no evidence has been found that would support the existence of yet unknown chemical mechanisms making a significant contribution to polar ozone loss. (4) Global modelling: results from process studies have been implemented in a prognostic chemistry climate model (CCM); simulations with improved parameterisations of processes relevant for polar ozone depletion are evaluated against satellite data and other long term records using data assimilation and detrended fluctuation analysis. Finally, measurements and process studies within RECONCILE were also applied to the winter 2010/11, when special meteorological conditions led to the highest chemical ozone loss ever observed in the Arctic. In addition to quantifying the 2010/11 ozone loss and to understand its causes including possible connections to climate change, its impacts were addressed, such as changes in surface ultraviolet (UV) radiation in the densely populated northern mid-latitudes.

Description: The mid-infrared FTIR-limb-sounder Michelson Interferometer for Passive Atmospheric Sounding – STRatospheric aircraft (MIPAS-STR) was deployed onboard the stratospheric aircraft M55 Geophysica during the RECONCILE campaign in the arctic winter/spring 2010. From the MIPAS-STR measurements, vertical profiles and 2-dimensional vertical cross-sections of temperature and trace gases are retrieved. Detailed mesoscale structures of polar vortex air, extra vortex air and vortex filaments are identified in the results at a typical vertical resolution of 1 to 2 km and typical horizontal sampling density of 45 or 25 km, depending on the sampling programme. Results are shown for the RECONCILE flight 11 on 2 March 2010 and are validated with collocated in-situ measurements of temperature, O3, CFC-11, CFC-12 and H2O. Exceptional agreement is found for the in-situ comparisons of temperature and O3, with mean differences (vertical profile/along flight track) of 0.2/−0.2 K for temperature and −0.01/0.05 ppmv for O3 and corresponding sample standard deviations of the mean differences of 0.7/0.6 K and 0.1/0.3 ppmv. The comparison of the retrieved vertical cross-sections of HNO3 from MIPAS-STR and the infrared limb-sounder Cryogenic Infrared Spectrometers and Telescopes for the Atmosphere – New Frontiers (CRISTA-NF) indicates comprehensive agreement. We discuss MIPAS-STR in its current configuration, the spectral and radiometric calibration of the measurements and the retrieval of atmospheric parameters from the spectra. The MIPAS-STR measurements are significantly affected by continuum-like contributions, which are attributed to background aerosol and broad spectral signatures from interfering trace gases and are important for mid-infrared limb-sounding measurements in the Upper Troposphere/Lower Stratosphere (UTLS) region. Considering for continuum-like effects, we present a scheme suitable for accurate retrievals of temperature and an extended set of trace gases, including the correction of a systematic line-of-sight offset.

Description: Vertical redistribution of HNO3 through condensation, sedimentation and evaporation of large HNO3-containing particles inside polar stratospheric clouds (PSCs) plays an important role in the chemistry of the Arctic winter stratosphere. In situ observations by the particle probe FSSP-100 during the RECONCILE campaign indicate unexpected large potential NAT (nitric acid trihydrate) particles inside PSCs. The observations can hardly be explained assuming particles with compact morphology and spherical shape due to limited growing time at temperatures below the existence temperature of NAT (TNAT). Utilizing simulations by the CLaMS and measurements by the airborne Fourier transform infrared spectrometer MIPAS-STR we study the impact of reduced settling velocities of NAT particles on vertical HNO3 redistribution. Reduced settling velocities are expected for spherical NAT particles with low mass density or aspheric NAT particles that might explain the maximum sizes of the particles observed in situ. The results of our study support the hypothesis that denitrification is produced by significantly aspheric (i.e. columnar) compact NAT particles which are characterised by reduced settling velocities.

Description: The mid-infrared FTIR-limb-sounder Michelson Interferometer for Passive Atmospheric Sounding–STRatospheric aircraft (MIPAS-STR) was deployed onboard the research aircraft M55 Geophysica during the RECONCILE campaign (Reconciliation of Essential Process Parameters for an Enhanced Predictability of Arctic Stratospheric Ozone Loss and its Climate Interactions) in the Arctic winter/spring 2010. From the MIPAS-STR measurements, vertical profiles and 2-dimensional vertical cross-sections of temperature and trace gases are retrieved. Detailed mesoscale structures of polar vortex air, extra vortex air and vortex filaments are identified in the results at typical vertical resolutions of 1 to 2 km and typical horizontal sampling densities of 45 or 25 km, depending on the sampling programme. Results are shown for the RECONCILE flight 11 on 2 March 2010 and are validated with collocated in-situ measurements of temperature, O3, CFC-11, CFC-12 and H2O. Exceptional agreement is found for the in-situ comparisons of temperature and O3, with mean differences (vertical profile/along flight track) of 0.2/−0.2 K for temperature and −0.01/0.05 ppmv for O3 and corresponding sample standard deviations of the mean differences of 0.7/0.6 K and 0.1/0.3 ppmv. The comparison of the retrieved vertical cross-sections of HNO3 from MIPAS-STR and the infrared limb-sounder Cryogenic Infrared Spectrometers and Telescopes for the Atmosphere–New Frontiers (CRISTA–NF) indicates a high degree of agreement. We discuss MIPAS-STR in its current configuration, the spectral and radiometric calibration of the measurements and the retrieval of atmospheric parameters from the spectra. The MIPAS-STR measurements are significantly affected by continuum-like contributions, which are attributed to background aerosol and broad spectral signatures from interfering trace gases, and are important for mid-infrared limb-sounding in the Upper Troposphere/Lower Stratosphere (UTLS) region. Taking into consideration continuum-like effects, we present a scheme suitable for accurate retrievals of temperature and an extended set of trace gases, including the correction of a systematic line-of-sight offset.

Description: The Gimballed Limb Observer for Radiance Imaging of the Atmosphere (GLORIA) is a prototype of an imaging Fourier Transform Spectrometer (FTS) for PREMIER, a former candidate mission for ESA's Earth Explorer 7. GLORIA is deployed on board various research aircraft such as the Russian M55 Geophysica or the German HALO. The instrument provides detailed infrared images of the Upper Troposphere/Lower Stratosphere (UTLS) region, which plays a crucial role in the climate system. GLORIA uses a two-dimensional detector array for infrared limb observations in emission and therefore needs large-area blackbody radiation sources (126 mm × 126 mm) for calibration. In order to meet the highly demanding uncertainty requirements for the scientific objectives of the GLORIA missions and due to the sophisticated tomographic evaluation scheme, the spatial distribution of the radiance temperature of the blackbody calibration sources has to be determined with an uncertainty of about 0.1 K. Since GLORIA is exposed to the hostile environment of the UTLS with mutable low temperature and pressure, an in-flight calibration system has to be carefully designed to cope with those adverse circumstances. The GLORIA in-flight calibration system consists of two identical weight-optimised high-precision blackbody radiation sources, which are independently stabilised at two different temperatures. The two point calibration is in the range of the observed atmospheric infrared radiance emissions with 10 K below and 30 K above ambient temperature, respectively. Thermo-Electric Coolers are used to control the temperature of the blackbody radiation sources offering the advantage of avoiding cryogens and mechanical coolers. The design and performance of the GLORIA in-flight calibration system is presented. The blackbody calibration sources have been comprehensively characterised for their spatially (full aperture) and spectrally (7 to 13 μm) resolved radiation properties in terms of radiance temperatures traceable to the International Temperature Scale (ITS-90) at the Physikalisch-Technische Bundesanstalt (PTB), the national metrology institute of Germany.

Description: The Gimballed Limb Observer for Radiance Imaging of the Atmosphere (GLORIA) is an imaging Fourier transform spectrometer that is capable of operating on various high-altitude research aircraft. It measures the atmospheric emission in the thermal infrared spectral region in limb and nadir geometry. GLORIA consists of a classical Michelson interferometer combined with an infrared camera. The infrared detector has a usable area of 128 × 128 pixels, measuring up to 16 384 interferograms simultaneously. Imaging Fourier transform spectrometers impose a number of challenges with respect to instrument calibration and algorithm development. The optical setup with extremely high optical throughput requires the development of new methods and algorithms for spectral and radiometric calibration. Due to the vast amount of data there is a high demand for scientifically intelligent optimisation of the data processing. This paper outlines the characterisation and processing steps required for the generation of radiometrically and spectrally calibrated spectra. Methods for performance optimisation of the processing algorithm are presented. The performance of the data processing and the quality of the calibrated spectra are demonstrated for measurements collected during the first deployments of GLORIA on aircraft.

Description: We report first chemistry mode retrieval results from the new airborne limb-imaging infrared FTS (Fourier transform spectrometer) GLORIA (Gimballed Limb Observer for Radiance Imaging of the Atmosphere) and comparisons with observations by the conventional airborne limb-scanning infrared FTS MIPAS-STR (Michelson Interferometer for Passive Atmospheric Sounding – STRatospheric aircraft). For GLORIA, the flights aboard the high-altitude research aircraft M55 Geophysica during the ESSenCe campaign (ESa Sounder Campaign 2011) were the very first in field deployment after several years of development. The simultaneous observations of GLORIA and MIPAS-STR during the flight on 16 December 2011 inside the polar vortex and under conditions of optically partially transparent polar stratospheric clouds (PSCs) provided us the first opportunity to compare the observations by two different infrared FTS generations directly. We validate the GLORIA results with MIPAS-STR based on the lower vertical resolution of MIPAS-STR and compare the vertical resolutions of the instruments derived from their averaging kernels. The retrieval results of temperature, HNO3, O3, H2O, CFC-11 and CFC-12 show reasonable agreement of GLORIA with MIPAS-STR and collocated in situ observations. For the horizontally binned hyperspectral limb images, the GLORIA sampling outnumbered the horizontal cross-track sampling of MIPAS-STR by up to 1 order of magnitude. Depending on the target parameter, typical vertical resolutions of 0.5 to 2.0 km were obtained for GLORIA and are typically a factor of 2 to 4 better compared to MIPAS-STR. While the improvement of the performance, characterization and data processing of GLORIA are the subject of ongoing work, the presented first results already demonstrate the considerable gain in sampling and vertical resolution achieved with GLORIA.