Ralf Sussmann

Long‐term trends of inorganic chlorine from ground‐based infrared solar spectra: Past increases and evidence for stabilization

Long-term time series of hydrogen chloride (HCl) and chlorine nitrate (ClONO2) total column abundances has been retrieved from high spectral resolution ground-based solar absorption spectra recorded with infrared Fourier transform spectrometers at nine NDSC (Network for the Detection of Stratospheric Change) sites in both Northern and Southern Hemispheres. The data sets span up to 24 years and most extend until the end of 2001. The time series of Cl-y (defined here as the sum of the HCl and ClONO2 columns) from the three locations with the longest time-span records show rapid increases until the early 1990s superimposed on marked day-to-day, seasonal and inter-annual variability. Subsequently, the buildup in Cl-y slows and reaches a broad plateau after 1996, also characterized by variability. A similar time evolution is also found in the total chlorine concentration at 55 km altitude derived from Halogen Occultation Experiment (HALOE) global observations since 1991. The stabilization of inorganic chlorine observed in both the total columns and at 55 km altitude indicates that the near-global 1993 organic chlorine (CCly) peak at the Earths surface has now propagated over a broad altitude range in the upper atmosphere, though the time lag is difficult to quantify precisely from the current data sets, due to variability. We compare the three longest measured time series with two-dimensional model calculations extending from 1977 to 2010, based on a halocarbon scenario that assumes past measured trends and a realistic extrapolation into the future. The model predicts broad Cl-y maxima consistent with the long-term observations, followed by a slow Cl-y decline reaching 12-14% relative to the peak by 2010. The data reported here confirm the effectiveness of the Montreal Protocol and its Amendments and Adjustments in progressively phasing out the major man-related perturbations of the stratospheric ozone layer, in particular, the anthropogenic chlorine-bearing source gases. (Less)

Methane retrievals from greenhouse gases observing satellite (GOSAT) shortwave infrared measurements: performance comparison of proxy and physics retrieval algorithms

We compare two conceptually different methods for determining methane column-averaged mixing ratios image from Greenhouse Gases Observing Satellite (GOSAT) shortwave infrared (SWIR) measurements. These methods account differently for light scattering by aerosol and cirrus. The proxy method retrieves a CO_2 column which, in conjunction with prior knowledge on CO_2 acts as a proxy for scattering effects. The physics-based method accounts for scattering by retrieving three effective parameters of a scattering layer. Both retrievals are validated on a 19-month data set using ground-based X_CH_4 at 12 stations of the Total Carbon Column Observing Network (TCCON), showing comparable performance: for the proxy retrieval we find station-dependent retrieval biases from −0.312% to 0.421% of X_CH_4 a standard deviation of 0.22% and a typical precision of 17 ppb. The physics method shows biases between −0.836% and −0.081% with a standard deviation of 0.24% and a precision similar to the proxy method. Complementing this validation we compared both retrievals with simulated methane fields from a global chemistry-transport model. This identified shortcomings of both retrievals causing biases of up to 1ings and provide a satisfying validation of any methane retrieval from space-borne SWIR measurements, in our opinion it is essential to further expand the network of TCCON stations.

Global CO2 fluxes inferred from surface air-sample measurements and from TCCON retrievals of the CO2 total column

We present the first estimate of the global distribution of CO_2 surface fluxes from 14 stations of the Total Carbon Column Observing Network (TCCON). The evaluation of this inversion is based on 1) comparison with the fluxes from a classical inversion of surface air-sample-measurements, and 2) comparison of CO_2 mixing ratios calculated from the inverted fluxes with independent aircraft measurements made during the two years analyzed here, 2009 and 2010. The former test shows similar seasonal cycles in the northern hemisphere and consistent regional carbon budgets between inversions from the two datasets, even though the TCCON inversion appears to be less precise than the classical inversion. The latter test confirms that the TCCON inversion has improved the quality (i.e., reduced the uncertainty) of the surface fluxes compared to the assumed or prior fluxes. The consistency between the surface-air-sample-based and the TCCON-based inversions despite remaining flaws in transport models opens the possibility of increased accuracy and robustness of flux inversions based on the combination of both data sources and confirms the usefulness of space-borne monitoring of the CO_2 column.

Lidar and numerical studies on the different evolution of vortex pair and secondary wake in young contrails

Vortex-regime evolution of contrails is investigated by focusing on the role of ambient humidity. Lidar cross-section measurements and observational analysis are combined with numerical simulations of fluid dynamics and microphysics. Contrail evolution behind four-turbofan aircraft is classified into three different scenarios. In the case of ice-subsaturated air, a visible pair of wingtip vortices is formed that disappears at the end of the vortex regime. In case of ice supersaturation, a diffuse secondary wake evolves above the wingtip vortices. It is due to detrainment of ice particles growing by sublimation of ambient humidity. A vertical wake-gap opens between the wingtip vortices and the secondary wake. It is due to subsaturated air moving upward along the outer edges of the sinking vortex tubes accumulating around the upper stagnation point of the vortex system. The vertical wake-gap preferably occurs in the wake of heavy (four turbofans) aircraft, since the vortices behind light aircraft migrate down too slowly. The secondary wake is composed of nonspherical particles larger than the ones in the wingtip vortices which are spherical particles and/or particles smaller than ≈0.5 μm. In most cases the secondary wake is the only part of a contrail that persists after vortex breakdown. This is because the ice in the vortex tubes evaporates due to adiabatic heating as the vortices travel downward. Only in the rare case of higher ambient ice supersaturation (>2%) do both parts of a contrail contribute to the persistent ice cloud. The number of ice crystals initially formed is typically reduced by a factor of 200 by evaporation (60% ambient humidity). This leads to a high population of interstitial particles. The results imply that formation of persistent contrails can be minimized by technical means.

Differences in early contrail evolution of two‐engine versus four‐engine aircraft: Lidar measurements and numerical simulations

Jet- and vortex-regime evolution of contrails behind cruising aircraft is investigated by focusing on the role of aircraft type. Cross-section measurements by ground-based lidar and observational analysis are combined with numerical simulations of fluid dynamics and microphysics in the wake of a two-engine aircraft. Depending on ambient humidity levels, contrail evolution behind short-/medium-range twin-turbofan airliners is classified into two scenarios, which is in contrast to the three scenarios observed for a wide-body four-turbofan aircraft. In the case of ice-subsaturated ambient air, a short visible contrail is formed behind a two-engine aircraft that disappears before the ice is fully entrained into the wingtip vortices (in most cases ≃ 4 s behind aircraft). The early evaporation of the ice is mainly due to the fast initial jet expansion, mixing the exhaust with the ambient air. Contrails behind a wide-body four-engine aircraft always survive at least until vortex breakdown (i.e., typically 2 min behind aircraft). This is simply due to the larger ice mass in the contrail because of the higher fuel flow rate. Generally, in the case of ice supersaturation, a diffuse secondary wake evolves above the primary vortex wake. For a two-engine aircraft, always the whole contrail persists, while for a four-engine aircraft, the ice inside the primary wake disappears in most cases after vortex breakdown, when the relative humidity is only slightly above ice saturation. In the more rare cases of higher ice-supersaturation the ice in the primary wake survives vortex breakdown and becomes part of the persistent contrail.

Strategy for high-accuracy-and-precision retrieval of atmospheric methane from the mid-infrared FTIR network

We present a strategy (MIR-GBM v1.0) for the retrieval of column-averaged dry-air mole fractions of methane (XCH4) with a precision<0.3 % (1-σ diurnal variation, 7-min integration) and a seasonal bias <0.14 % from mid-infrared ground-based solar FTIR measurements of the Network for the Detection of Atmospheric Composition Change (NDACC, comprising 22 FTIR stations). This makes NDACC methane data useful for satellite validation and for the inversion of regional-scale sources and sinks in addition to long-term trend analysis. Such retrievals complement the high accuracy and precision near-infrared observations of the younger Total Carbon Column Observing Network (TCCON) with time series dating back 15 years or so before TCCON operations began. MIR-GBM v1.0 is using HITRAN 2000 (including the 2001 update release) and 3 spectral micro windows (2613.70–2615.40 cm −1, 2835.50–2835.80 cm −1, 2921.00– 2921.60 cm−1). A first-order Tikhonov constraint is applied to the state vector given in units of per cent of volume mixing ratio. It is tuned to achieve minimum diurnal variation without damping seasonality. Final quality selection of the retrievals uses a threshold for the goodness of fit ( χ2 < 1) as well as for the ratio of root-mean-square spectral noise and information content ( <0.15 %). Column-averaged dryair mole fractions are calculated using the retrieved methane profiles and four-times-daily pressure-temperature-humidity profiles from National Center for Environmental Prediction (NCEP) interpolated to the time of measurement. MIR-GBM v1.0 is the optimum of 24 tested retrieval strategies (8 different spectral micro-window selections, 3 spectroscopic line lists: HITRAN 2000, 2004, 2008). Dominant errors of the non-optimum retrieval strategies are Correspondence to: R. Sussmann (ralf.sussmann@kit.edu) systematic HDO/H2O-CH4 interference errors leading to a seasonal bias up to ≈5 %. Therefore interference errors have been quantified at 3 test sites covering clear-sky integrated water vapor levels representative for all NDACC sites (Wollongong maximum = 44.9 mm, Garmisch mean = 14.9 mm, Zugspitze minimum = 0.2 mm). The same quality ranking of the 24 strategies was found for all 3 test sites with one optimum, i.e. MIR-GBM v1.0. Seasonality of XCH4 above the Zugspitze (47 ◦ N) shows a minus-sine shape with a minimum in March/April, a maximum in September, and an amplitude of 16.2 ± .9 ppb (0.94± 0.17 %). This agrees well with the WFM-DOAS v2.0 scientific XCH4 retrieval product. A conclusion from this paper is that improved spectroscopic parameters for CH 4, HDO, and H2O in the 2613– 2922 cm−1 spectral domain are urgently needed. If such become available with sufficient accuracy, at least two more spectral micro windows could be utilized leading to another improvement in precision. The absolute inter-calibration of NDACC MIR-GBM v1.0 XCH4 to TCCON data is subject of ongoing work.

Vertical dispersion of an aircraft wake: Aerosol‐lidar analysis of entrainment and detrainment in the vortex regime

Vertical dispersion of contrails in the vortex regime is investigated by focusing on the role of entrainment and detrainment of exhaust with respect to the pair of trailing vortices. A ground-based backscatter-depolarization lidar with an integrated CCD camera provides information on optical and geometrical parameters of the contrail in the time span between 5.7 and 50.3 s behind a B747-400 aircraft. This is combined with coincident airborne in situ measurements of turbulence and the vertical profiles of temperature and wind speed in a case study. The two wingtip vortices, separated by 47 m, are descending with an increasing speed (2.5-3.1 m/s for 10.8-47.8 s behind aircraft) in the weakly non-stably-stratified atmosphere. The turbulent vertical dissipation rate on the day of the study above southern Germany is a factor of 1000 higher than found typically above oceans at cruising altitude. At 4.2 s behind the aircraft, a diffuse secondary wake starts to evolve above the two wingtip vortices. After 50 s the secondary wake encloses a cross-sectional area (4410 m 2 ) comparable to that of the primary wake (4620 m 2 ) and a relative ice surface area of 1:5. The observed early onset of the secondary wake is conjectured to be due to turbulent detrainment of fluid out of the primary wake which can be enhanced by detrainment due to baroclinic forces later in the vortex regime evolution. By exclusion of other mechanisms of secondary wake formation, detrainment of fluid from the primary wake is concluded to be the precondition for secondary wake formation. Detrainment due to baroclinic forces, shear or turbulence is, in general, unlikely to be absent for typical atmospheric conditions. It is suggested that the ambient humidity level may determine when a secondary wake is visible above a vortex pair and when it is not.

On seasonality of stratomesospheric CO above midlatitudes: New insight from solar FTIR spectrometry at Zugspitze and Garmisch

[1] A significant seasonality in stratomesospheric CO (24―100 km) above mid-latitudes is derived from FTIR via a new regularization scheme. Half hourly means from the Zugspitze (47.42°N, 10.98°E, 2964 m a.s.l.) and nearby Garmisch (745 m a.s.l.) measurements show excellent agreement (R = 0.94, slope 0.91, standard deviation 12%). Mean seasonality ofthe Zugspitze series (1999―2008) shows a November- April enhancement (February maximum 3.63 x 10 16 cm ―2 ) and a summer background (1.64 x 10 16 cm ―2 ) which agrees with the WACCM model. Measured monthly means reveal a year-to-year variability of up to 32% (1-sigma) in winter not reproduced by WACCM (R = ―0.13). Frequency distributions of daily means are right skewed in winter due to enhancements by vortex air transport (1―3 days duration) which typically reflect CO levels of the vortex border and may even reach vortex-center levels (≈300% of the multi-annual monthly median).

Global land mapping of satellite-observed CO2 total columns using spatio-temporal geostatistics

ABSTRACT This study presents an approach for generating a global land mapping dataset of the satellite measurements of CO2 total column (XCO2) using spatio-temporal geostatistics, which makes full use of the joint spatial and temporal dependencies between observations. The mapping approach considers the latitude-zonal seasonal cycles and spatio-temporal correlation structure of XCO2, and obtains global land maps of XCO2, with a spatial grid resolution of 1° latitude by 1° longitude and temporal resolution of 3 days. We evaluate the accuracy and uncertainty of the mapping dataset in the following three ways: (1) in cross-validation, the mapping approach results in a high correlation coefficient of 0.94 between the predictions and observations, (2) in comparison with ground truth provided by the Total Carbon Column Observing Network (TCCON), the predicted XCO2 time series and those from TCCON sites are in good agreement, with an overall bias of 0.01 ppm and a standard deviation of the difference of 1.22 ppm and (3) in comparison with model simulations, the spatio-temporal variability of XCO2 between the mapping dataset and simulations from the CT2013 and GEOS-Chem are generally consistent. The generated mapping XCO2 data in this study provides a new global geospatial dataset in global understanding of greenhouse gases dynamics and global warming.

The exploitation of ground-based Fourier transform infrared observations for the evaluation of tropospheric trends of greenhouse gases over Europe

Abstract Solar absorption measurements using Fourier transform infrared (FTIR) spectrometry carry information about the atmospheric abundances of many constituents, including non-CO2 greenhouse gases. Such observations have regularly been made for many years as a contribution to the Network for the Detection of Stratospheric Change (NDSC). They are the only ground-based remote sensing observations available nowadays that carry information about a number of greenhouse gases in the free troposphere. This work focuses on the discussion of the information content of FTIR long-term monitoring data of some direct and indirect greenhouse gases (CH4, N2O, O3 and CO and C2H6, respectively), at six NDSC stations in Western Europe. This European FTIR network covers the polar to subtropical regions. At several stations of the network, the observations span more than a decade. Existing spectral time series have been reanalyzed according to a common optimized retrieval strategy, in order to derive distinct tropospheric and stratospheric abundances for the above-mentioned target gases. A bootstrap resampling method has been implemented to evaluate trends of the tropospheric burdens of the target gases, including their uncertainties. In parallel, simulations of the target time series are being made with the Oslo CTM2 model: comparisons between the model results and the observations provide valuable information to improve the model and, in particular, to optimize emission estimates that are used as inputs to the model simulations. The work is being performed within the EC project UFTIR. The paper focuses on N2O for which the first trend results have been obtained.