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Die vorliegende Arbeit beschäftigt sich mit der Produktion positiv und negativ geladener Pionen im System Au+Au bei einer kinetischen Strahlenergie von 1,5 GeV pro Nukleon. Diese Daten wurden im Juli 1998 mit dem Kaonenspektrometer KaoS gemessen. Es liegen Pi-Minus-Spektren bei drei verschiedenen Laborwinkeln (Theta Lab = 40°, 48°, 60°) vor sowie Pi-Plus-Spektren bei fünf Laborwinkeln(Theta Lab = 32°, 40°, 48°, 60°, 71,5°). Die Spektren können als Funktion der Energie im Nukleon-Nukleon-Schwerpunktssystem mit der Summe zweier Boltzmannverteilungen beschrieben werden, deren Steigung sich ebenso wie der unter Annahme isotroper Emission im Schwerpunktssytem integrierte Wirkungsquerschnitt mit dem Laborwinkel ändert. Als mögliche Ursache dieses Verhaltens wird untersucht, ob eine polare Anisotropie der Emission vorliegt. Eine solche wurde in früheren Experimenten [49, 50] für die Pionenproduktion in Proton-Proton-Stößen gefunden und als Effekt der p-Wellen-Produktion von Pionen interpretiert, bei der als Zwischenschritt eine Resonanz, zumeist eine Delta-Resonanz, angeregt wird. Die Zerfallskinematik dieser Resonanzen bewirkt duch ihren Drehimpuls eine Winkelverteilung der emittierten Pionen [24]. In Kern-Kern-Stößen führt die Abschattung von Pionen durch nicht an der Reaktion teilnehmende Nukleonen zu einer zusätzlichen Richtungsabhängigkeit der Emission. Unter der Annahme, daß Energie- und Winkelabhängigkeit separierbar sind, wird in einem einfachen Modell der Winkelanteil des differentiellen Wirkungsquerschnitts als Funktion des Kosinus des Schwerpunktswinkels mit einer Parabelform beschrieben. Um den Anpassungsparameter a2, der die Stäke der Anisotropie quantifiziert, zu ermitteln, stehen zwei Methoden zur Verfügung, die simultane Anpassung der bei festem Laborwinkel gemessenen Spektren und der Vergleich mit einer durch Schnitte durch die Laborimpulsspektren erzeugten Verteilung bei Theta cm = 90°. Beide Verfahren ermitteln erfolgreich den Anisotropieparameter aus in einer Monte-Carlo-Simulation erzeugten Spektren mit parabelförmiger Winkelverteilung. Die mit beiden Methoden ermittelten a2-Werte stimmen für Pi+ wie für Pi- im Rahmen der Fehler überein. Die Winkelverteilung der Pi+ ist mit a2 = 0,7 +- 0,1 stärker ausgeprägt als die der Pi- mit a2 = 0,4 +- 0,1, beide werden bevorzugt unter Theta cm = 0° und Theta cm = 180° emittiert. Allerdings zeigt sich in beiden Methoden eine starke Abhängigkeit von der Phasenraumabdeckung der Daten und beide sind nicht geeignet, eine Abhängigkeit des Anisotropieparameters von der Pionenenergie zu ermitteln....
Excitation functions for quasi-elastic scattering have been measured at backward angles for the systems 32,34S+197Au and 32,34S+208Pb for energies spanning the Coulomb barrier. Representative distributions, sensitive to the low energy part of the fusion barrier distribution, have been extracted from the data. For the fusion reactions of 32,34S with 197Au couplings related to the nuclear structure of 197Au appear to be dominant in shaping the low energy part of the barrier distibution. For the system 32S+208Pb the barrier distribution is broader and extends further to lower energies, than in the case of 34S+208Pb. This is consistent with the interpretation that the neutron pick-up channels are energetically more favoured in the 32S induced reaction and therefore couple more strongly to the relative motion. It may also be due to the increased collectivity of 32S, when compared with 34S.
We report the first measurements of 1,1,1,2,3,3,3-heptafluoropropane (HFC-227ea), a substitute for ozone depleting compounds, in remote regions of the atmosphere and present evidence for its rapid growth. Observed mixing ratios ranged from below 0.01 ppt in deep firn air to 0.59 ppt in the northern mid-latitudinal upper troposphere. Firn air samples collected in Greenland were used to reconstruct a history of atmospheric abundance. Year-on-year increases were deduced, with acceleration in the growth rate from 0.026 ppt per year in 2000 to 0.057 ppt per year in 2007. Upper tropospheric air samples provide evidence for a continuing growth until late 2009. Fur- thermore we calculated a stratospheric lifetime of 370 years from measurements of air samples collected on board high altitude aircraft and balloons. Emission estimates were determined from the reconstructed atmospheric trend and suggest that current "bottom-up" estimates of global emissions for 2005 are too high by more than a factor of three.
We report the first measurements of 1,1,1,2,3,3,3-heptafluoropropane (HFC-227ea), a substitute for ozone depleting compounds, in air samples originating from remote regions of the atmosphere and present evidence for its accelerating growth. Observed mixing ratios ranged from below 0.01 ppt in deep firn air to 0.59 ppt in the current northern mid-latitudinal upper troposphere. Firn air samples collected in Greenland were used to reconstruct a history of atmospheric abundance. Year-on-year increases were deduced, with acceleration in the growth rate from 0.029 ppt per year in 2000 to 0.056 ppt per year in 2007. Upper tropospheric air samples provide evidence for a continuing growth until late 2009. Furthermore we calculated a stratospheric lifetime of 370 years from measurements of air samples collected on board high altitude aircraft and balloons. Emission estimates were determined from the reconstructed atmospheric trend and suggest that current "bottom-up" estimates of global emissions for 2005 are too high by a factor of three.
The CARIBIC (Civil Aircraft for the Regular Investigation of the Atmosphere Based on an Instrument Container) passenger aircraft observatory performed in situ measurements at 10–12 km altitude in the South Asian summer monsoon anticyclone between June and September 2008. These measurements enable us to investigate this atmospheric region, which so far has mostly been observed from satellites, using the broad suite of trace gases and aerosols measured by CARIBIC. Elevated levels of a range of atmospheric pollutants were recorded e.g. carbon monoxide, total reactive nitrogen oxides, aerosol particles and several volatile organic compounds. The measurements provide detailed information about the chemical composition of air in different parts of the monsoon anticyclone, particularly of ozone precursors. While covering a range of 3500 km inside the monsoon anticyclone, CARIBIC observations show remarkable consistency, i.e. with regular latitudinal patterns of trace gases during the entire monsoon period. Trajectory calculations indicate that these air masses originated mainly from South Asia and Mainland Southeast Asia.
Using the CARIBIC trace gas and aerosol measurements in combination with the Lagrangian particle dispersion model FLEXPART we investigated the characteristics of monsoon outflow and the chemical evolution of air masses during transport. Estimated photochemical ages of the air were found to agree well with transport times from a source region east of 95 ° E. The photochemical ages of the air in the southern part of the monsoon anticyclone were consistently younger (less than 7 days) and the air masses mostly in an ozone forming chemical regime. In its northern part the air masses were older (up to 13 days) and had unclear ozone formation or destruction potential. Based on analysis of forward trajectories several receptor regions were identified. In addition to predominantly westward transport, we found evidence for efficient transport (within 10 days) to the Pacific and North America, particularly during June and September, and also of cross-tropopause exchange, which was strongest during June and July. Westward transport to Africa and further to the Mediterranean was the main pathway during July.
The CARIBIC (Civil Aircraft for the Regular Investigation of the Atmosphere Based on an Instrument Container) passenger aircraft observatory performed in situ measurements at 10–12 km altitude in the South Asian summer monsoon anticyclone between June and September 2008. These measurements enable us to investigate this atmospheric region (which so far has mostly been observed from satellites) using the broad suite of trace gases and aerosol particles measured by CARIBIC. Elevated levels of a variety of atmospheric pollutants (e.g. carbon monoxide, total reactive nitrogen oxides, aerosol particles, and several volatile organic compounds) were recorded. The measurements provide detailed information about the chemical composition of air in different parts of the monsoon anticyclone, particularly of ozone precursors. While covering a range of 3500 km inside the monsoon anticyclone, CARIBIC observations show remarkable consistency, i.e. with distinct latitudinal patterns of trace gases during the entire monsoon period.
Using the CARIBIC trace gas and aerosol particle measurements in combination with the Lagrangian particle dispersion model FLEXPART, we investigated the characteristics of monsoon outflow and the chemical evolution of air masses during transport. The trajectory calculations indicate that these air masses originated mainly from South Asia and mainland Southeast Asia. Estimated photochemical ages of the air were found to agree well with transport times from a source region east of 90–95° E. The photochemical ages of the air in the southern part of the monsoon anticyclone were systematically younger (less than 7 days) and the air masses were mostly in an ozone-forming chemical mode. In its northern part the air masses were older (up to 13 days) and had unclear ozone formation or destruction potential. Based on analysis of forward trajectories, several receptor regions were identified. In addition to predominantly westward transport, we found evidence for efficient transport (within 10 days) to the Pacific and North America, particularly during June and September, and also of cross-tropopause exchange, which was strongest during June and July. Westward transport to Africa and further to the Mediterranean was the main pathway during July.
In late 2013, a whole air flask collection programme was started at Taunus Observatory (TO) in central Germany. Being a rural site in close proximity to the Rhine–Main area, Taunus Observatory allows assessment of emissions from a densely populated region. Owing to its altitude of 825 m, the site also regularly experiences background conditions, especially when air masses approach from north-westerly directions. With a large footprint area mainly covering central Europe north of the Alps, halocarbon measurements at the site have the potential to improve the database for estimation of regional and total European halogenated greenhouse gas emissions. Flask samples are collected weekly for offline analysis using a GC/MS system simultaneously employing a quadrupole as well as a time-of-flight mass spectrometer. As background reference, additional samples are collected approximately once every 2 weeks at the Mace Head Atmospheric Research Station (MHD) when air masses approach from the site's clean air sector. Thus the time series at TO can be linked to the in situ AGAGE measurements and the NOAA flask sampling programme at MHD. An iterative baseline identification procedure separates polluted samples from baseline data. While there is good agreement of baseline mixing ratios between TO and MHD, with a larger variability of mixing ratios at the continental site, measurements at TO are regularly influenced by elevated halocarbon mixing ratios. Here, first time series are presented for CFC-11, CFC-12, HCFC-22, HFC-134a, HFC-227ea, HFC-245fa, and dichloromethane. While atmospheric mixing ratios of the chlorofluorocarbons (CFCs) decrease, they increase for the hydrochlorofluorocarbons (HCFCs) and the hydrofluorocarbons (HFCs). Small unexpected differences between CFC-11 and CFC-12 are found with regard to frequency and relative enhancement of high mixing ratio events and seasonality, although production and use of both compounds are strictly regulated by the Montreal Protocol, and therefore a similar decrease in atmospheric mixing ratios should occur. Dichloromethane, a solvent about which recently concerns have been raised regarding its growing influence on stratospheric ozone depletion, does not show a significant trend with regard to both baseline mixing ratios and the occurrence of pollution events at Taunus Observatory for the time period covered, indicating stable emissions in the regions that influence the site. An analysis of trajectories from the Hybrid Single Particle Lagrangian Integrated Trajectory (HYSPLIT) model reveals differences in halocarbon mixing ranges depending on air mass origin.
In late 2013, a whole air flask collection program started at the Taunus Observatory (TO) in central Germany. Being a rural site in close vicinity to the densely populated Rhein-Main area, Taunus Observatory allows to assess local and regional emissions. Owed to its altitude of 825 m, the site also regularly experiences background conditions, especially when air masses approach from north-westerly directions. With a large footprint area mainly covering central Europe north of the Alps, halocarbon measurements at the site have the potential to improve the data base for estimation of regional and total European halogenated greenhouse gas emissions. Flask samples are collected weekly for offline analysis using a GC-MS system employing a quadrupole as well as a time-of-flight mass spectrometer. As background reference, additional samples are collected approximately bi-weekly at the Mace Head Atmospheric Research Station (MHD) when air masses approach from the site’s clean air sector. Thus the TO time series can be linked to the in-situ AGAGE measurements and the NOAA flask sampling program at MHD. An iterative baseline identification procedure separates polluted samples from baseline data. While there is good agreement of baseline mixing ratios between TO and MHD, with a larger variability of mixing ratios at the continental site, measurements at TO are regularly influenced by elevated halocarbon mixing ratios. Here, first time series are presented for CFC-11, CFC-12, HCFC-22, HFC-134a, HFC-227ea, HFC-245fa, and dichloromethane. While atmospheric mixing ratios of the CFCs decrease, they increase for the HCFC and the HFCs. Small unexpected differences between CFC-11 and CFC-12 are found with regard to the occurrence of high mixing ratio events and seasonality, although production and use of both compounds are strictly regulated by the Montreal Protocol, and therefore a similar decrease of atmospheric mixing ratios should occur. Dichloromethane, a solvent about which recently concerns have risen regarding its growing influence on stratospheric ozone depletion, does not show a significant trend with regard to both, baseline mixing ratios and the occurrence of pollution events at Taunus Observatory for the time period covered, indicating stable emissions in the regions that influence the site. An analysis of HYSPLIT trajectories reveals differences in halocarbon mixing ranges depending on air mass origin.
We present novel measurements of five short-lived brominated source gases (CH2Br2, CHBr3, CH2ClBr, CHCl2Br and CHClBr2) obtained using a gas chromatograph-mass spectrometer system on board the High Altitude and Long Range Research Aircraft (HALO). The instrument is extremely sensitive due to the use of chemical ionisation, allowing detection limits in the lower parts per quadrillion (10-15) range. Data from three campaigns using the HALO aircraft are presented, where the Upper Troposphere/Lower Stratosphere (UTLS) of the Northern Hemisphere mid to high latitudes were sampled during winter and during late summer to early fall. We show that an observed decrease with altitude in the stratosphere is consistent with the relative lifetimes of the different compounds. Distributions of the five source gases and total organic bromine just below the tropopause shows an increase in mixing ratio with latitude, in particular during polar winter. This increase in mixing ratio is explained by increasing lifetimes at higher latitudes during winter. As the mixing ratio at the extratropical tropopause are generally higher than those derived for the tropical tropopause, extratropical troposphere-to-stratosphere transport will result in elevated levels of organic bromine in comparison to air transported over the tropical tropopause. The observations are compared to model estimates using different emission scenarios. A scenario which has emissions most strongly concentrated to low latitudes cannot reproduce the observed latitudinal distributions and will tend to overestimate bromine input through the tropical tropopause from CH2Br2 and CHBr3. Consequently, the scenario also overestimates the amount of brominated organic gases in the stratosphere. The two scenarios with the highest overall emissions of CH2Br2 tend to overestimate mixing ratios at the tropical tropopause but are in much better agreement with extratropical tropopause values, showing that not only total emissions but also latitudinal distributions in the emissions are of importance. While an increase in tropopause values with latitude is reproduced with all emission scenarios during winter, the simulated extratropical tropopause values are on average lower than the observations during late summer to fall. We show that a good knowledge of the latitudinal distribution of tropopause mixing ratios and of the fractional contributions of tropical and extratropical air is needed to derive stratospheric inorganic bromine in the lowermost stratosphere from observations. Depending on the underlying emission scenario, differences of a factor 2 in reactive bromine derived from observations and model outputs are found for the lowermost stratosphere, based on source gas injection. We conclude that a good representation of the contributions of different source regions is required in models for a robust assessment of the role of short-lived halogen source gases on ozone depletion in the UTLS.
Stability of halocarbons in whole air samples from the upper
troposphere and lowermost stratosphere
(2019)
Measurements of halogenated hydrocarbons of ambient air frequently rely on canister sampling followed by offline laboratory analysis. This allows for a large number of compounds to be analysed under stable conditions, maximising measurement precision. However, individual compounds might be affected during storage of canister samples. In order to assess halocarbon stability in whole air samples from the upper troposphere and lowermost stratosphere, we performed stability tests using the air sampling unit High REsolution Sampler (HIRES) which is part of the CARIBIC (Civil Aircraft for the Regular Investigation of the Atmosphere Based on an Instrument Container) instrument package. HIRES holds 88 light-weight stainless steel cylinders that are pressurized in flight to 4.5 bar using metal bellows pumps. The HIRES sampling unit was first deployed in 2010, but has up to now not been used for regular halocarbon analysis with exception of chloromethane. The sample collection unit was tested for sampling and storage effects of 28 halogenated compounds. The focus was on compound stability in the stainless steel canisters during storage of up to five weeks and on the influence of ozone, since flights take place in the upper troposphere and lowermost stratosphere with ozone mixing ratios of up to several hundred ppbV. Most of the investigated (hydro)chlorofluorocarbons and long-lived hydrofluorocarbons were found to be stable over a storage time of up to five weeks and were unaltered by ozone being present during pressurization. Some compounds such as for example dichloromethane, trichloromethane and tetrachloroethene started to decrease in the canisters after a storage time of more than two weeks or exhibited lowered mixing ratios in samples pressurized with ozone present. Few compounds such as for example tetrachloromethane and tribromomethane were found to be not stable in the HIRES stainless-steel canisters independent of ozone levels. Also growth was observed during storage, namely for HFC-152a and HFC-23.