ALBERT

Description: Direct measurements of OH and HO2 over a tropical rainforest were made for the first time during the GABRIEL campaign in October 2005, deploying the custom-built HORUS instrument (HydrOxyl Radical measurement Unit based on fluorescence Spectroscopy), adapted to fly in a Learjet wingpod. Biogenic hydrocarbon emissions were expected to strongly reduce the OH and HO2 mixing ratios as the air is transported from the ocean over the forest. However, surprisingly high mixing ratios of both OH and HO2 were encountered in the boundary layer over the rainforest. The HORUS instrumentation and calibration methods are described in detail and the measurement results obtained are discussed. The extensive dataset collected during GABRIEL, including measurements of many other trace gases and photolysis frequencies, has been used to quantify the main sources and sinks of OH. Comparison of these measurement-derived formation and loss rates of OH indicates strong previously overlooked recycling of OH in the boundary layer over the tropical rainforest, occurring in chorus with isoprene emission.

Description: As a major source region of the hydroxyl radical OH, the Tropics largely control the oxidation capacity of the atmosphere on a global scale. However, emissions of hydrocarbons from the tropical rainforest that react rapidly with OH can potentially deplete the amount of OH and thereby reduce the oxidation capacity. The airborne GABRIEL field campaign in equatorial South America (Suriname) in October 2005 investigated the influence of the tropical rainforest on the HOx budget (HOx=OH+HO2). The first observations of OH and HO2 over a tropical rainforest are compared to steady state concentrations calculated with the atmospheric chemistry box model MECCA. The important precursors and sinks for HOx chemistry, measured during the campaign, are used as constraining parameters for the simulation of OH and HO2. Significant underestimations of HOx are found by the model over land during the afternoon, with mean ratios of observation to model of 12.2±3.5 and 4.1±1.4 for OH and HO2, respectively. The discrepancy between measurements and simulation results is correlated to the abundance of isoprene. While for low isoprene mixing ratios (above ocean or at altitudes 〉3 km), observation and simulation agree fairly well, for mixing ratios 〉200 pptV (

Description: The detection of nitric acid trihydrate (NAT, HNO3×3H2O) particles in the tropical transition layer (TTL) harmonizes our understanding of polar stratospheric cloud formation. Large reactive nitrogen (NOy) containing particles were observed on 8 August 2006 by instruments onboard the high altitude research aircraft M55-Geophysica near and below the tropical tropopause. The particles, most likely NAT, have diameters less than 6 μm and concentrations below 10−4 cm−3. The NAT particle layer was repeatedly detected at altitudes between 15.1 and 17.5 km over extended areas of 9.5 to 17.2° N and 1.5° W to 2.7° E above the African continent. Satellite observations suggest that the NAT particles could have nucleated on ice fed by convective activity. Once nucleated, the NAT particles can slowly grow within the TTL for days, while being transported over long distances. Their in-situ detection combined with global model simulations of the NAT supersaturation near the tropical tropopause indicate the potential for a tropical tropopause NAT particle belt.

Description: A statistical analysis for the comparability of water (H2O) and ozone (O3) data sets sampled during the SPURT aircraft campaigns and the MOZAIC passenger aircraft flights is presented. The Kolmogoroff–Smirnoff test reveals that the distribution functions from SPURT and MOZAIC trace gases differ from each other with a confidence of 95%. A variance analysis shows a different variability character in both trace gas data sets. While the SPURT data only contain atmospheric processes variable on a diurnal or synoptical timescale, MOZAIC data also reveal processes, which vary on inter-seasonal and seasonal timescales. The SPURT data set does not represent the full MOZAIC H2O variance in the UT/LS for climatological investigations, whereas the variance of O3 is much better represented. SPURT H2O data are better suited in the stratosphere, where the MOZAIC RH sensor looses its sensitivity.

Description: In the tropics, deep convection is the major source of uncertainty in water vapor transport to the upper troposphere and into the stratosphere. Although accurate measurements in this region would be of first order importance to better understand the processes that govern stratospheric water vapor concentrations and trends in the context of a changing climate, they are sparse because of instrumental shortcomings and observational challenges. Therefore, the Falcon research aircraft of the Deutsches Zentrum für Luft- und Raumfahrt (DLR) flew a zenith-viewing water vapor differential absorption lidar (DIAL) during the Tropical Convection, Cirrus and Nitrogen Oxides Experiment (TROCCINOX) in 2004 and 2005 in Brazil. The measurements were performed alternatively on three water vapor absorption lines of different strength around 940 nm. These are the first aircraft DIAL measurements in the tropical upper troposphere and in the mid-latitudes lower stratosphere. A sensitivity analysis reveals that the DIAL profiles have an accuracy of ~5% between altitudes of 8 and 16 km. This is confirmed by intercomparisons with the Fast In-situ Stratospheric Hygrometer (FISH) and the Fluorescent Advanced Stratospheric Hygrometer (FLASH) onboard the Russian M-55 Geophysica research aircraft during five coordinated flights. The average relative differences between FISH and DIAL amount to –3%±8% and between FLASH and DIAL to –8%±14%, negative meaning DIAL is more humid. The average distance between the probed air masses was 129 km. The DIAL is found to have no altitude- or latitude-dependent bias. A comparison with the balloon ascent of a laser absorption spectrometer gives an average difference of 0%±19% at a distance of 75 km. Six tropical DIAL under-flights of the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) on board ENVISAT show a mean difference of –8%±49% at an average distance of 315 km. While the comparison with MIPAS is somewhat less significant due to poorer comparison conditions, the agreement with the in-situ hygrometers provides evidence of the excellent quality of FISH, FLASH and DIAL. Most DIAL profiles exhibit a smooth exponential decrease of water vapor mixing ratio in the tropical upper troposphere to lower stratosphere transition. The hygropause with a minimum mixing ratio of ~2.5 μmol/mol is found between 15 and 16 km, 1 to 2 km beneath the local tropopause. A high-resolution (2 km horizontal, ~200 m vertical) DIAL cross section through the anvil outflow of tropical convection shows that the ambient humidity is increased by a factor of three across 100 km.

Description: We present the validation of a water vapour dataset obtained by the Airborne Microwave Stratospheric Observing System AMSOS, a passive microwave radiometer operating at 183 GHz. Vertical profiles are retrieved from spectra by an optimal estimation method. The useful vertical range lies in the upper troposphere up to the mesosphere with an altitude resolution of 8 to 16 km and a horizontal resolution of about 57 km. Flight campaigns were performed once a year from 1998 to 2006 measuring the latitudinal distribution of water vapour from the tropics to the polar regions. The obtained profiles show clearly the main features of stratospheric water vapour in all latitudinal regions. Data are validated against a set of instruments comprising satellite, ground-based, airborne remote sensing and in-situ instruments. It appears that AMSOS profiles have a dry bias of 3–20%, when compared to satellite experiments. A good agreement with a difference of 3.3% was found between AMSOS and in-situ hygrosondes FISH and FLASH and an excellent matching of the lidar measurements from the DIAL instrument in the short overlap region in the upper troposphere.

Description: We have developed a Lagrangian air-parcel cirrus model (LACM), to diagnose the processes controlling water in the tropical tropopause layer (TTL). LACM applies parameterised microphysics to air parcel trajectories. The parameterisation includes the homogeneous freezing of aerosol droplets, the growth/sublimation of ice particles, and sedimentation of ice particles, so capturing the main dehydration mechanism for air in the TTL. Rehydration is also considered by resetting the water vapour mixing ratio in an air parcel to the value at the point in the 4-D analysis/forecast data used to generate the trajectories, but only when certain conditions, indicative of convection, are satisfied. These conditions are imposed to confine what processes contribute to rehydration. The conditions act to restrict rehydration of the Lagrangian air parcels to regions where convective transport of water vapour from below is significant, at least to the extent that the analysis/forecast captures this process. The inclusion of hydration and dehydration mechanisms in LACM results in total water fields near tropical convection that have more of the "stripey" character of satellite observations of high cloud, than do either the ECMWF analysis or trajectories without microphysics. The mixing ratios of total water in the TTL, measured by a high-altitude aircraft over Brazil (during the TROCCINOX campaign), have been reconstructed by LACM using trajectories generated from ECMWF analysis. Two other Lagrangian reconstructions are also tested: linear interpolation of ECMWF analysed specific humidity onto the aircraft flight track, and instantaneous dehydration to the saturation vapour pressure over ice along trajectories. The reconstructed total water mixing ratios along aircraft flight tracks are compared with observations from the FISH total water hygrometer. Process-oriented analysis shows that modelled cirrus cloud events are responsible for dehydrating the air parcels coming from lower levels, resulting in total water mixing ratios as low as 2 μmol/mol. Without adding water back to some of the trajectories, the LACM and instantaneous-dehydration reconstructions have a dry bias. The interpolated-ECMWF reconstruction does not suffer this dry bias, because convection in the ECMWF model moistens air parcels dramatically, by pumping moist air upwards. This indicates that the ECMWF model captures the gross features of the rehydration of air in the TTL by convection. Overall, the ECMWF models captures well the exponential decrease in total water mixing ratio with height above 250 hPa, so that all the reconstruction techniques capture more than 75% of the variance in the measured total water mixing ratios over the depth of the TTL. We have therefore developed a simple method for re-setting the total water in LACM using the ECMWF-analysed specific humidity in regions where the model predicts convection. By picking up the main contributing processes to dehydration and rehydration in the TTL, LACM reconstructs total water mixing ratios along aircraft flight tracks at the top of the TTL, close to the cold point, that are always in substantially better agreement with observations than instantaneous-dehydration reconstructions, and better than the ECMWF analysis for regions of high relative humidity and cloud.

Description: We present a comparison of different Lagrangian and steady state box model runs with measurement data obtained during the GABRIEL campaign over the tropical Atlantic Ocean and the rainforest in the Guyanas, October 2005. Lagrangian modelling of boundary layer (BL) CO constrained by measurements of reactive trace gases and radiation is used to derive a horizontal gradient (≈5.6 pmol/mol km−1) of this compound from the ocean to the rainforest (east to west). This is significantly smaller than that derived from the measurements (16–48 pmol/mol km−1), indicating that photochemical production from organic precursors alone cannot explain the observed strong gradient. It appears that HCHO is overestimated by the Lagrangian and "steady state" models, which include dry deposition but not exchange with the free troposphere (FT). The relatively short lifetime of HCHO (50–100 min) implies substantial BL-FT exchange. The mixing-in of FT air affected by African and South American biomass burning at an estimated rate of 0.12 h−1 increases the CO and lowers the HCHO mixing ratios, leading to a better agreement with measurements. A 24 h mean deposition velocity of 1.35 cm/s for H2O2 over the ocean as well as over the rainforest is deduced assuming BL-FT exchange adequate to the results for CO. The measured increase of the organic peroxides from the ocean to the rainforest (≈0.66 nmol/mol d−1) is significantly overestimated by the Lagrangian model, even when using high values for the deposition velocity and the entrainment rate. Our results point at either heterogeneous loss of organic peroxides and/or their radical precursors or a missing reaction path of peroxy radicals not forming peroxides in isoprene chemistry. We calculate a mean integrated daytime net ozone production (NOP) in the BL of (0.2±5.9) nmol/mol (ocean) and (2.4±2.1) nmol/mol (rainforest). The NOP strongly correlates with NO and shows a positive tendency in the boundary layer over the rainforest.

Description: 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 the vertical tracers profiles, relative vertical tracers gradients, and tracer-tracer relationships in the tropical Upper Troposphere/Lower Stratosphere (UT/LS), using tropopause coordinates. Observations come from the four tropical campaigns performed from 1998 to 2006 with the research aircraft Geophysica and have been directly compared to the output of the ECHAM5/MESSy CCM. The model vertical resolution in the TTL allows for appropriate comparison with high-resolution aircraft observations and the diagnostics used highlight common TTL features between the model and the observational data. 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 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-O3 and H2O-O3 scatter plots and of the Probability Distribution Function (PDF) of the H2O-O3 pair completes this picture as it allows to better distinguish tropospheric and stratospheric regimes that can be identified, first, by their differing chemical composition. The joint analysis and comparison of observed and modelled data allows us to evaluate the capability of the model in reproducing the observed vertical structure of the TTL and its variability, and also to assess whether observations from particular regions on a monthly timescale can be representative of the fine scale mean structure of the Tropical Tropopause Layer.

Description: During SPURT (Spurenstofftransport in der Tropopausenregion, trace gas transport in the tropopause region) we performed measurements of a wide range of trace gases with different lifetimes and sink/source characteristics in the northern hemispheric upper troposphere (UT) and lowermost stratosphere (LMS). A large number of in-situ instruments were deployed on board a Learjet 35A, flying at altitudes up to 13.7 km, at times reaching to nearly 380 K potential temperature. Eight measurement campaigns (consisting of a total of 36 flights), distributed over all seasons and typically covering latitudes between 35° N and 75° N in the European longitude sector (10° W–20° E), were performed. Here we present an overview of the project, describing the instrumentation, the encountered meteorological situations during the campaigns and the data set available from SPURT. Measurements were obtained for N2O, CH4, CO, CO2, CFC12, H2, SF6, NO, NOy, O3 and H2O. We illustrate the strength of this new data set by showing mean distributions of the mixing ratios of selected trace gases, using a potential temperature-equivalent latitude coordinate system. The observations reveal that the LMS is most stratospheric in character during spring, with the highest mixing ratios of O3 and NOy and the lowest mixing ratios of N2O and SF6. The lowest mixing ratios of NOy and O3 are observed during autumn, together with the highest mixing ratios of N2O and SF6 indicating a strong tropospheric influence. For H2O, however, the maximum concentrations in the LMS are found during summer, suggesting unique (temperature- and convection-controlled) conditions for this molecule during transport across the tropopause. The SPURT data set is presently the most accurate and complete data set for many trace species in the LMS, and its main value is the simultaneous measurement of a suite of trace gases having different lifetimes and physical-chemical histories. It is thus very well suited for studies of atmospheric transport, for model validation, and for investigations of seasonal changes in the UT/LMS, as demonstrated in accompanying and elsewhere published studies.