Highly resolved observations of trace gases in the lowermost stratosphere and upper troposphere from the Spurt project: an overview

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

Highly resolved observations of trace gases in the lowermost stratosphere and upper troposphere from the Spurt project: an overview

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

Long-term in situ measurements of NOx and NOy at Jungfraujoch 1998–2009: time series analysis and evaluation

We present an analysis of the NOy (NOx + other oxidized species) measurements at the high alpine site Jungfraujoch (JFJ, 3580 m a.s.l.) for the period 1998–2009, which is the longest continous NOy data set reported from the lower free troposphere worldwide. Due to stringent emission control regulations, nitrogen oxides (NOx) emissions have been reduced significantly in Europe since the late 1980s as well as during the investigation period. However, the time series of NOy at JFJ does not show a consistent trend but a maximum during 2002 to 2004 and a decreasing tendency thereafter. The seasonal cycle of NOy exhibits a maximum in the warm season and a minimum in the cold months, opposite to measurements in the PBL, reflecting the seasonal changes in vertical transport and mixing. Except for summer, the seasonal mean NOx concentrations at JFJ show a high year-to-year variability which is strongly controlled by short episodic pollution events obscuring any long-term trends. The low variability in mean and median NOx values in summer is quite remarkable indicating rapid photochemical conversion of NOx to higher oxidized species (NOz) of the NOy family on a timescale shorter than the time required to transport polluted air from the boundary layer to JFJ. In order to evaluate the quality of the NOy data series, an in-situ intercomparison with a second collocated NOy analyzer with a separate inlet was performed in 2009–2010 which showed an overall agreement within 10% including all uncertainties and errors.ISSN:1680-7375ISSN:1680-736

Analysis of elevated springtime levels of Peroxyacetyl nitrate (PAN) at the high Alpine research sites Jungfraujoch and Zugspitze

The largest atmospheric peroxyacetyl nitrate (PAN) mole fractions at remote surface sites in the Northern Hemisphere are commonly observed during the months April and May. Different formation mechanisms for this seasonal maximum have previously been suggested: hemispheric-scale production from precursors accumulated during the winter months, increased springtime transport from up-wind continents or increased regional-scale production in the atmospheric boundary layer from recent emissions. The two high Alpine research sites Jungfraujoch (Switzerland) and Zugspitze (Germany) exhibit a distinct and consistent springtime PAN maximum. Since these sites intermittently sample air masses of free-tropospheric and boundary layer origin, they are ideally suited to identify the above-mentioned PAN formation processes and attribute local observations to these. Here we present a detailed analysis of PAN observations and meteorological conditions during May 2008 when PAN levels were especially elevated at both sites. The highest PAN concentrations were connected with anticyclonic conditions, which persisted in May 2008 for about 10 days with north-easterly advection towards the sites. A backward dispersion model analysis showed that elevated PAN concentrations were caused by the combination of favourable photochemical production conditions and large precursor concentrations in the European atmospheric boundary layer. The results suggest that the largest PAN values in spring 2008 at both sites were attributable to regional-scale photochemical production of PAN in the (relatively cold) planetary boundary layer from European precursors, whereas the contribution of inter-continental transport or free-tropospheric build-up was of smaller importance for these sites.ISSN:1680-7375ISSN:1680-736

Particle backscatter and relative humidity measured across cirrus clouds and comparison with microphysical cirrus modelling

Advanced measurement and modelling techniques are employed to estimate the partitioning of atmospheric water between the gas phase and the condensed phase in and around cirrus clouds, and thus to identify in-cloud and out-of-cloud supersaturations with respect to ice. In November 2008 the newly developed balloon-borne backscatter sonde COBALD (Compact Optical Backscatter and AerosoL Detector) was flown 14 times together with a CFH (Cryogenic Frost point Hygrometer) from Lindenberg, Germany (52° N, 14° E). The case discussed here in detail shows two cirrus layers with in-cloud relative humidities with respect to ice between 50% and 130%. Global operational analysis data of ECMWF (roughly 1° × 1° horizontal and 1 km vertical resolution, 6-hourly stored fields) fail to represent ice water contents and relative humidities. Conversely, regional COSMO-7 forecasts (6.6 km × 6.6 km, 5-min stored fields) capture the measured humidities and cloud positions remarkably well. The main difference between ECMWF and COSMO data is the resolution of small-scale vertical features responsible for cirrus formation. Nevertheless, ice water contents in COSMO-7 are still off by factors 2–10, likely reflecting limitations in COSMO's ice phase bulk scheme. Significant improvements can be achieved by comprehensive size-resolved microphysical and optical modelling along backward trajectories based on COSMO-7 wind and temperature fields, which allow accurate computation of humidities, homogeneous ice nucleation, resulting ice particle size distributions and backscatter ratios at the COBALD wavelengths. However, only by superimposing small-scale temperature fluctuations, which remain unresolved by the numerical weather prediction models, can we obtain a satisfying agreement with the observations and reconcile the measured in-cloud non-equilibrium humidities with conventional ice cloud microphysics. Conversely, the model-data comparison provides no evidence that additional changes to ice-cloud microphysics – such as heterogeneous nucleation or changing the water vapour accommodation coefficient on ice – are required.ISSN:1680-7375ISSN:1680-736

Balloon-borne match measurements of midlatitude cirrus clouds

Observations of high supersaturations with respect to ice inside cirrus clouds with high ice water content (> 0.01 g kg−1) and high crystal number densities (> 1 cm−3) are challenging our understanding of cloud microphysics and of climate feedback processes in the upper troposphere. However, single measurements of a cloudy air mass provide only a snapshot from which the persistence of ice supersaturation cannot be judged. We introduce here the "cirrus match technique" to obtain information about the evolution of clouds and their saturation ratio. The aim of these coordinated balloon soundings is to analyze the same air mass twice. To this end the standard radiosonde equipment is complemented by a frost point hygrometer, "SnowWhite", and a particle backscatter detector, "COBALD" (Compact Optical Backscatter AerosoL Detector). Extensive trajectory calculations based on regional weather model COSMO (Consortium for Small-Scale Modeling) forecasts are performed for flight planning, and COSMO analyses are used as a basis for comprehensive microphysical box modeling (with grid scale of 2 and 7 km, respectively). Here we present the results of matching a cirrus cloud to within 2–15 km, realized on 8 June 2010 over Payerne, Switzerland, and a location 120 km downstream close to Zurich. A thick cirrus cloud was detected over both measurement sites. We show that in order to quantitatively reproduce the measured particle backscatter ratios, the small-scale temperature fluctuations not resolved by COSMO must be superimposed on the trajectories. The stochastic nature of the fluctuations is captured by ensemble calculations. Possibilities for further improvements in the agreement with the measured backscatter data are investigated by assuming a very slow mass accommodation of water on ice, the presence of heterogeneous ice nuclei, or a wide span of (spheroidal) particle shapes. However, the resulting improvements from these microphysical refinements are moderate and comparable in magnitude with changes caused by assuming different regimes of temperature fluctuations for clear-sky or cloudy-sky conditions, highlighting the importance of proper treatment of subscale fluctuations. The model yields good agreement with the measured backscatter over both sites and reproduces the measured saturation ratios with respect to ice over Payerne. Conversely, the 30% in-cloud supersaturation measured in a massive 4 km thick cloud layer over Zurich cannot be reproduced, irrespective of the choice of meteorological or microphysical model parameters. The measured supersaturation can only be explained by either resorting to an unknown physical process, which prevents the ice particles from consuming the excess humidity, or – much more likely – by a measurement error, such as a contamination of the sensor housing of the SnowWhite hygrometer by a precipitation drop from a mixed-phase cloud just below the cirrus layer or from some very slight rain in the boundary layer. This uncertainty calls for in-flight checks or calibrations of hygrometers under the special humidity conditions in the upper troposphere.ISSN:1680-7375ISSN:1680-736

Highly resolved observations of trace gases in the lowermost stratosphere and upper troposphere from the Spurt project: an overview

ISSN:1680-7375ISSN:1680-736