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The present study was elaborated within the scope of the INTAFERE (Integrated Analysis of Mobile Organic Foreign Substances in Rivers) project which investigates the occurrence of xenobiotics in small freshwater streams with particular consideration of social impact factors. The aim of this study is to investigate the seasonal and spatial variance of organic micropollutants in small fresh water streams and to identify possible sources and sinks. Therefore four small freshwater river systems in Hesse, Germany, have been investigated with respect to common organic pollutants such as: the organophosphates tri-n-butyl phosphate (TBP), tris(2-butoxyethyl)phosphate (TBEP), tris(2-chloroethyl)phosphate (TCEP), tris(1-chloro-2-propyl)phosphate (TCPP), and tris(1,3-dichloro-2-propyl)phosphate (TDCPP), the synthetic musk fragrances 1,3,4,6,7,8-hexahydro-4,6,6,7,8,8-hexa-methylcyclopenta-[g]-2-benzopyran (HHCB) and 7-acetyl-1,1,3,4,4,6-hexamethyl-1,2,3,4-tetrahydronaphthalene (AHTN), the endocrine disruptors bisphenol A (BPA), 4-tert-octylphenol (OP) and the technical isomer mixture of 4-nonylphenol (NP), the herbicide terbutryn [2-(t-butylamino)-4-(ethylamino)-6-(methylthio)-s-triazine] as well as the insect repellent N,N-diethyl-m-toluamide (DEET). Water samples were collected in the time span from September 2003 to September 2006 at 26 sampling locations. The samples were extracted with solid phase extraction (SPE) and analyzed by coupled gas chromatography-mass spectrometry (GC-MS). For quantification the internal standard method was used. The results of the study showed an ubiquitous occurrence of organic pollutants in the fresh water streams of the study area. The organophosphates have been detected in 90 % of the water samples with mean concentrations of 502 ng/l (TCPP), 276 ng/l (TBP), 183 ng/l (TBEP), 118 ng/l (TCEP) and 117 ng/l (TDCPP). Sewage treatment plant (STP) effluents were identified as the dominating source for the chlorinated organophosphates as well as for the synthetic musk fragrances and the insect repellent DEET in the river systems. Consequently the highest concentrations were observed in the Schwarzbach system characterized by the highest proportion of waste water compared to the other river systems. Mean concentration levels of the synthetic musk fragrances HHCB and ATHN were 141 ng/l and 46 ng/l, respectively and 124 ng/l in case of DEET. The synthetic musk fragrances showed a clear seasonal trend with significantly lower concentrations in summer times compared to winter times, which is ascribed to stronger photodegradation and volatization during summer times. In contrast, mean DEET concentrations and loads were significantly higher in summer than in autumn, winter and spring, in parallel with the main insect season. The concentrations of the endocrine disruptors BPA, NP and OP in the river water samples ranged from <20 ng/l to 1927 ng/l, <10 ng/l to 770 ng/l, and <10 ng/l to 420 ng/l, respectively. Whereas OP was present in about 2/3 of the samples, NP and BPA could only be detected in 56% and 13% of the water samples, respectively. BPA levels exceeded in two samples the predicted no-effect concentration (PNEC) for water organisms. In case of NP, highest concentrations and loads were found in September 2003 and decreased significantly since then. In contrast, concentrations and loads of OP which serves in a similar application field remained nearly constant during the sampling period. The decrease of NP can be attributed to the implementation of the European Directive 2003/53/EG, which restricts the use of nonylphenols and nonylphenol ethoxylates since January 2005. However, at the end of the sampling period in September 2006, NP could still be detected at mean concentrations of 18 ng/l in the river waters of the sampling area. Furthermore, absence of NP in several samples from associated STP effluents indicate that the STPs cannot be the only sources for NP found in the river water. The herbicide terbutryn was present in the rivers during the whole sampling period from September 2003 to September 2006 despite a ban on its use as a herbicide from January 2004 on. Terbutryn levels ranged from < 4 ng/l to 5600 ng/l, showing a clear spatial pattern with high terbutryn concentrations in the Weschnitz and Modau river systems and significantly lower terbutryn levels in Schwarzbach and Winkelbach. Results from the analysis of two STP effluents discharging into the Weschnitz and the Modau, respectively, indicate that terbutryn enters the rivers from this source. Furthermore, terbutryn concentrations and loads showed a clear seasonal trend with significantly higher levels in summer and autumn. Obviously, the ban on agricultural use of terbutryn at the end of 2003 had no discernable influence on terbutryn concentration in the rivers because there was no trend of decreasing.
Recently, carbonates have attracted a lot of attention, due to the recognition of their importance in the global carbon cycle. This was enabled by improvement of the experimental techniques that allow for investigating the stability, structure, and physical properties of materials and high-pressures and high-temperatures, that is, they allow for investigating minerals and geochemical processes at the conditions occurring deep inside Earth. Although a lot of research has been focused on carbonates, there are still some open questions regarding their structure and physical properties at such extreme conditions. The aim of this thesis is to establish a deeper understanding of the nature of the phase transitions in carbonates by studying how do the atoms building up the crystal structure vibrate, that is lattice dynamics. The methodology adapted in this study is a combination of experimental and computational methods which allows for a very thorough examination of the problem. The computational approach allows to determine parameters that are elusive or tedious to measure, and the experimental results provide a solid benchmark for the calculations. This tandem of methods has been widely used for investigating lattice dynamics of various materials. In this study it was used to elucidate the structure and properties of carbonates in the deep Earth conditions
The TTL is the transition layer between the tropical troposphere and stratosphere, and is the main region where tropospheric air enters the stratosphere. In this thesis different transport processes are studied by using in situ measurements of tracers. Long-lived tracers were measured with the High Altitude Gas Analyzer (HAGAR) on board the M55 Geophysica aircraft. The instrument was developed by the University of Frankfurt and measures the long-lived tracers CO2, N2O, CFC-12, CFC-11, H-1211, SF6, CH4 and H2 with two gas chromatographic channels and a CO2 sensor (LICOR). The measurements are supported by CO and O3 measurements of other instruments. Two campaigns were conducted to obtain measurements in the TTL: SCOUT-O3 (November/December 2005 in Darwin, Australia) and AMMA-SCOUT-O3 (August 2006 in Ouagadougou, Burkina Faso). After a general introduction of the thesis in chapters one and two, the third chapter describes the findings during this last campaign. Five local flights are analyzed to study the different transport processes that occur in the tropical tropopause layer above West-Africa: deep convection up to the level of main convective outflow, vertical mixing after overshooting of air in deep convection, horizontal inmixing from the extratropical lower stratosphere, and horizontal transport across the subtropical barrier. Main findings are that the TTL over West-Africa is mostly influenced by remote convection. The subtropical barrier is not a strong barrier but more a region of transition between the extratropical and the tropical stratosphere. Chapter 4 presents the results obtained during the SCOUT-O3 campaign. From the eight local flights the last four flights (051129, 051130a, 051130b, 051205) show enhanced values of ozone, CO and CO2 between 355 and 380 K potential temperature in comparison with the first four flights (051116, 051119, 051123, 051125). Horizontal inmixing from the extra-tropical stratosphere and influence of the local convective system Hector cannot explain the enhanced values of the two flights on 30 November Therefore, other possible explanations for these enhanced CO, CO2 and ozone levels are proposed. The first explanation is vertical mixing in the vicinity of the jet stream. However, the jet cannot explain the differences between the flights on 30 November and the flights on 29 November and 5 December. Another possible explanation is influence of polluted boundary layer air masses from the Indonesian region. Especially air sampled during the flights on November 30 crossed large parts of northern Indonesia between 8 and 10 days before the measurements. Convective uplift of biomass burning and other pollution plumes can transport CO and ozone precursors into the upper troposphere, where they can significantly enhance the ozone production. The last chapter deals with the vertical ascent rate in the TTL and uses measurements of both the SCOUT-O3 and AMMA-SCOUT-O3 campaign as well as data from previous aircraft campaigns (TROCCINOX and APE-THESEO). Time scales and residence times for mean vertical transport in the background TTL are estimated for different seasons and over different geographic regions using in situ observations of CO2 and long-lived tracers. The vertical transport time scales are constrained using the seasonal variation of CO2 in the tropical troposphere as a “tracer clock” for vertical ascent. Two methods are applied to calculate the residence time in the layer between 360 and 390 K potential temperature. The first method uses the slope of the CO2 index, the second method fits the CO2 index directly to the measurements assuming a constant ascent rate. The first method yields residence times for Australia,West Africa, and Brazil of the same order, 35-45 days to 380 K and 50 days to 390 K (where no value can be derived for Australia as the slope is changing approximately one month before the campaign). For APE-THESEO, the method does not yield reasonable results. The best estimates using the second method show moderate residence times between 360 and 390 K of 60±25 days SCOUT-O3 (NH autumn) and 43±8 days for AMMA/SCOUT-O3 (NH summer). These results agree well with the results calculated using the first method. For APE-THESEO and TROCCINOX the best fits yield shorter residence times of 23±7 and 40±10 days, respectively, both during winter. These results correspond well to the expectations based on the seasonal variation of the Brewer-Dobson circulation.
Melt segregation inside the earth consists of two different processes: 1) Generation of partially molten rock and 2) separation of melt, produced from partially molten rock, from the solid residual matrix. This thesis focuses on the later process. The 2 phase flow dynamics combines the study of flow dynamics of melt and matrix. Several studies have given the background theoretical frameworks for the flow dynamics of melt inside the earth. [McKenzie, 1984] summarizes the studies of [Ahern and Turcotte, 1979; Frank, 1968; Sleep, 1975] and gives a complete set of governing equations for the 2-phase flow problem.
[Bercovici et al., 2001] gives a general formulation considering the univariate system of equations related to matrix and melt flow which includes the interfacial surface force. The assumption of melt having negligible viscosity compare to the matrix has been abandoned. Therefore, based on these formulations, we have constructed our numerical model and thereafter a fortran code PERCOL2D to get an insight of melt percolation process through porous media. Additionally, we have used the Helmhotz decomposition, which splits a smooth and rapidly decaying vector field into an irrotational vector field and an incompressible vector field [Srámek, 2007], for matrix and fluid viscosity in order to lower the number of linearly independent variables to minimize the computational complications. The melt residing at inter-granular areas of lithosphere, forms an interconnected network even at low porosity. Therefore, being less dense than the matrix, melt moves up through porous media due to its buoyancy. Compaction of matrix, which occurs to compensate the melt separation, is considered in this thesis, where the effective bulk and shear viscosity of matrix are function of melt fraction. We have effective bulk viscosity of matrix as inversely proportional to melt fraction. Porosity dependence of effective bulk and shear viscosity leads to stronger melt focusing in highly porous region like mid ocean ridges [Katz, 2008] since the ratio of bulk and shear viscosity is smaller (< 10) than the constant viscosity case for the porous waves having non dimensional amplitude 5% or higher. Moreover, it is observed in [Richard et al., 2012] that the solitary wave formed in porosity dependent viscous matrix settings are steeper than the one formed in the constant matrix viscosity setting.
Firstly some 1D numerical experiments with PERCOL2D have been carried out using fixed and periodic boundary conditions for zero source term (i.e. no melting or no freezing) and negligible surface tension.
3 series of model setups with different initial conditions have been carried out varying the width, non-dimensional amplitude and the background porosity value of the initial input of porous wave.
A mathematical derivation for 1D solitary wave solution for the two phase flow through porosity dependent compacting media, is obtained in this thesis which is different than the study of [Barcilon and Lovera, 1989; Barcilon and Richter, 1986; Scott and Stevenson, 1984; Spiegelman, 1993a,b] as the effective viscosity of matrix is constant there.
Although [Simpson and Spiegelman, 2011] gives the solitary wave solutions in 1D, 2D and 3D considering the porosity dependent effective viscosity of the matrix, but using the small background porosity approximation, they neglect the background porosity (i.e φ0) and therefore the effect of variation of compaction lengths, which causes variation in the shape and dynamics of the solitary wave. Therefore, the study [This thesis, Richard et al., 2012] can be used for more general purpose. Solitary waves in varying viscous medium, are steeper (cf fig.5.1) compared to the one in constant viscous medium and their speed decreases as an inverse function of the background porosity. Additionally, this analytical solution is used in our code PERCOL2D and also in FDCON for numerical benchmarking (1D) of PERCOL2D.
The role of melt grain contiguity is considered in the revised viscosity formulation [Schmeling et al., 2012] based on elastic moduli theory of a fluid filled poro-elastic medium. This formulation is used in this thesis to produce a comparative dispersion relationship between speed of the wave and the non dimensional amplitude of porous wave, based on both the viscosity formulations (fig. 6.20) where one can see that the model based on [Bercovici et al., 2001] formulation, converges to the same dispersion relationship obtained from [Simpson and Spiegelman, 2011]. Whereas, the dispersion relationship using [Schmeling et al., 2012] formulations, shows time-dependent decrease of phase velocity with increasing amplitude and it is not yet clear that whether these solutions converge to steady state porosity waves before the porosity becomes 1.
The present PhD thesis comprises structural geology, petrographic and geochronological investiga-tions on crystalline rocks of the Uppermost Unit in the southern Aegean realm. Studies were carried out in three areas: (1) on the island of Anafi, (2) in the area west of Melambes in central Crete and (3) between the villages of Pefkos, Kalami and Sykologos in the municipality of Viannos in eastern Crete.
The Uppermost Unit forms together with the underlying, non-metamorphic Pindos Unit the upper nappe system of the Cretan nappe pile that, unlike the units of the lower nappe system, was not affected by Late Oligocene to Early Miocene subduction-related metamorphism. The upper nappe system must therefore have been at upper levels of the lithosphere in the Late Oligocene. This is of particular im-portance when reconstructing the tectonometamorphic evolution of the Uppermost Unit. The Upper-most Unit is very heterogeneous in composition and is subdivided into several subunits, which differ mainly in their lithological composition and the degree of metamorphic overprint. Usually, it is subdi-vided into several low-grade metamorphic subunits and one high-grade metamorphic subunit. Within the scope of this PhD thesis, three of these subunits were examined; (1) the anchimetamorphic Arvi Unit, (2) the newly described Greenschist Unit and (3) the Asterousia Crystalline Complex (ACC).
The analyses conducted during this PhD thesis include: (1) structural geology investigations in the field, (2) microstructural and petrographic analyses on thin sections, (3) radiometric dating of zircons using isotope dilution thermal ionisation mass spectrometry (ID-TIMS) and laser ablation inductively coupled plasma mass spectrometry (LA-ICP-MS), (4) electron microprobe (EMP) analysis, (5) quartz texture analysis using electron-backscattered diffraction (EBSD), (6) semiquantitative analysis of min-eral phases using X-ray powder diffraction (XRD), (7) analysis of the modal composition of intrusive rocks applying point counting on thin sections and (8) X-ray microtomography (micro-CT) on chias-tolite hornfels.
...
Until now, the NW Indian Ocean was sparsely covered with coral proxy records, and records from the Maldives Archipelago do not exist. The first such coral proxy record from the central Maldives is presented in this study. It originates from a massive Porites lutea (Quoy and Gaimard, 1833) colony that was sampled March 2007 in the lagoon of Rasdhoo Atoll (4°N/ 73°W), which is located in the central Maldives. The record spans a period of 90 yrs and reaches back to 1917 AD with monthly to bimonthly resolution. This study investigates temporal variations of the skeletal stable oxygen (delta18O) and carbon (delta13C) isotopes, the strontium-to-calcium (Sr/Ca), and the annual extension-rates, and their relationship to historical climate variations 1917-2007. Annual extension-rates show an increase over the 20th century, and are correlated with instrumental sea surface temperatures (SST). The interannual variation of the extension-rates within 2.5-4 years is driven by the El Niño-Southern Oscillation (ENSO). The amount of skeletal extension during the summer months is triggered by variations in the strength of the SW monsoon. Interannual and decadal variability in monsoon current activity (18-19 yrs) and rainfall over India are an expression of the summer monsoon strength. This is the reason why a statistical link between coral extension-rates and precipitation over India can be established. This implies that annual extension-rates in corals can be used as a new proxy for Indian monsoon variability on decadal resolution. The delta18O record exhibits the 20th century warming trend that is influenced by the effect of monsoon-induced cooling. delta18O also reveals interannual ENSO triggered variability, which is due to ENSO-forced variations in SST and sea surface salinity (SSS). A decadal variation at 12-14 yrs cannot be linked to SST variations in the NW Indian Ocean, but with decadal variations of SSS. They could be caused by ENSO- forced variations of the monsoon currents during the mature phase of ENSO teleconnections in the Indian Ocean in boreal winter. The Sr/Ca record does not indicate a significant warming, in spite of the observed SST rise at the sampling site. Changes in seawater Sr/Ca cannot be excluded. Nevertheless, interannual ENSO forcing is still evident. Evidence for the Pacific Decadal Oscillation (PDO) is found during 1917-1955. Afterwards, the Sr/Ca data indicate the disappearance of PDO forcing. By the combination of Sr/Ca and delta18O it is possible to detect ~80% of historical El Niño and La Niña events at the sample site. This study confirms the notion that interannual to multi-decadal climate fluctuations in the Pacific play a crucial role for climate variability in the Indian Ocean.
The aim of this study is a better understanding of radiation processes in regional climate models (RCMs) in order to quantify their impact and to reduce possible errors. A first important task in finding an answer to this question was to examine the accuracy of the components of the radiation budget in regional climate simulations. To this end, the simulated radiation budgets of two regional climate simulations for Europe were compared with a satellite-based reference. In the simulations with the RCM COSMO-CLM there were some serious under- and overestimations of short- and long-wave net radiation in Europe. However, taking into account the differences in the reference datasets, the results of the COSMO-CLM were quite satisfactory.
Using statistical methods, the influence of potential sources of uncertainties was estimated. Uncertainties in the cloud cover and surface albedo had a significant impact on uncertainties in short-wave net radiation, the explained variance of uncertainties in cloud cover was two to three times higher than that of uncertainties in surface albedo. Uncertainties in the cloud cover resulted in significant errors in the net long-wave radiation. However, the influence of uncertainties in soil temperature on errors in the long-wave radiation budget was low or even negligible. These results were confirmed in a comparison with simulations of the REMO and ALADIN regional climate models. It is reasonable to expect that a better parameterization of relatively simple parameters such as cloud cover and surface albedo is a means of significantly improving the simulation of radiation budget components in the COSMO-CLM.
An important question for the application of RCMs is to examine whether the results of radiation uncertainties and their impact factors are comparable if the model is applied in a region that is not the one for which it was originally created. Comparisons of the simulated radiation budgets of different RCMs for West Africa showed that problems in the simulation of short- and long-wave radiation fluxes were a widespread problem. Most of the tested models showed some considerable under- or overestimation of the short- and long-wave radiation fluxes.
Similar to Europe uncertainties in cloud cover were also in the simulations for Africa a significant factor affecting uncertainties in the simulated radiation fluxes. However, for the African simulations uncertainties in the parameterization of surface albedo were much more important than in Europe. On average, overland uncertainties in the cloud cover and surface albedo were of similar importance. Uncertainties in soil temperature simulations were of higher importance in Africa, and reached overland similar values of the mean explained variance (R2 ≈ 0.2) such as uncertainties in the cloud cover. This indicates a geographical dependence of the model error. This study confirmed the assumption that an improved parameterization of relatively simple parameters such as the surface albedo in RCMs leads to a significant improvement in the modeled radiation budget, particularly in Africa.
The influence of errors in the simulated radiation budget components on the simulation of climate processes, such as the West-African monsoon (WAM), was investigated in a next step. The evaluation of ERA-Interim and ECHAM5 driven COSMO-CLM simulations for Africa showed that the main features of the WAM were well reproduced by the model, but there were only slight improvements compared to the driving data. The index of convective activity in the model simulations was much too high and precipitation was underestimated in large parts of tropical Africa. The partly considerable differences between the ERA-Interim and ECHAM5 driven simulations demonstrated the sensitivity of the RCM to the boundary conditions and in particular to the sea surface temperature. An excessive northwards shift of the monsoon in the model was influenced by the land-sea temperature gradient and the strength of the Saharan heat low. Consequently, a part of the error was due to the driving data and the model itself produced another part.
By modifying the parameterization of the bare soil albedo the errors in the radiation budget and 2 m temperature in the Sahara region were significantly reduced. Similarly, the overesti-mation of precipitation and convection has been reduced in the Sahel. The effect of this modifi-cation on the examined WAM area was low. This confirmed that especially in desert regions, errors in the surface albedo were a driving factor for errors in the radiation budget. However, there are other important factors not yet sufficiently understood that have a strong influence on the quality of the simulation of the WAM.
The analysis of the actual state, the quantification of error sources and the highlighting of connections made it possible to find means to reduce uncertainties in the simulated radiation in RCMs and to have a better understanding of radiation processes. However, the magnitude of the errors found, the number of possible influencing factors, and the complexity of interactions, indicate that there is still a need for further research in this area.
Cenozoic lignite deposits are widespread across Europe, Asia, America, Australia, and Indonesia. These deposits were the subject of numerous studies on changes in regional/global paleoclimates, paleobotany, paleoenvironment, and basin evolutions, which led to the formation of these lignites. In some of these Cenozoic lignite deposit basins, a succession of pale and dark lignite layers has been described in the Miocene Lower Rhine Basin in Germany, the Oligo-Miocene Gippsland Basin in southeastern Australia, and several Mio-Pliocene basins in southwestern China. Furthermore, pale and dark lithotypes in lignite seams also have been found in some Pliocene lignite deposit basins from Slovenia, Serbia, and Poland. The widespread cyclic occurrence of pale and dark layers in lignite basins might represent alternating depositional conditions related to the changes in plant communities, the regional/global climate, the tectonic setting, the Asian monsoon, and orbital periodicity during peat formation. ...
Over the last several decades, spinel-structured minerals with the chemical formula AB2O4 (where A and B stand for divalent and trivalent cations, respectively) have attracted more and more attention, particularly with regards to their breakdown at high pressures and temperatures and the nature of the so-called "post-spinel" phases. Spinel-structured phases with different endmember compositions, like magnetite (Fe3O4), hercynite (FeAl2O4) or spinel (MgAl2O4), are known to breakdown differently at high pressure-temperature conditions (e.g., Akaogi et al. 1999; Schollenbruch et al. 2010; Woodland et al. 2012). Such phases are of particular interest when they incorporate ferric (Fe3+) and ferrous (Fe2+) cations as this makes their stability sensitive to redox conditions. Since magnetite and magnesioferrite (MgFe3+ 2O4) have been found as inclusions in diamond (e.g., Stachel et al. 1998; Harte et al. 1999; Wirth et al. 2014; Palot et al. 2016; Jacob et al. 2016), understanding their phase relations is important for setting constraints on the conditions of their formation.
This study aimed to experimentally investigate the phase relations of Fe-Mg spinel-structured phases at conditions of the deep upper mantle and transition zone. Exploring the stability of new post-spinel phases and their characterization were also major goals of this study. Approaching a pyrolitic mantle composition by adding amounts of SiO2 in the system allowed constraints on the relevance of Fe-Mg post-spinel phases coexisting with mantle silicates to be made. ...
Die vorliegende Arbeit liefert einen Beitrag zum Verständnis der Rolle des RO x bei der troposphärischen Ozonbildung. Troposphärisches Ozon (O 3 ) spielt eine wichtige Rolle bei der Selbstreinigung der Atmosphäre. Andererseits führen erhöhte Ozonkonzentrationen zu gesundheitlichen Beeinträchtigungen beim Menschen und Schäden an Pflanzen und Umwelt. Die Anwesenheit von flüchtigen organischen Verbindungen (VOCs) führt zur Bildung von Peroxyradikalen (RO x ), die das normale photochemische Gleichgewicht zwischen Ozon und Stickoxiden zu Gunsten erhöhter OzonKonzentrationen verschieben. Im Rahmen der Arbeit wurde ein chemischer Verstärker zur Messung der GesamtPeroxyradikalkonzentration gebaut. RO x reagiert im Einlass des Gerätes mit hinzugefügtem NO und CO in einer Kettenreaktion und bildet dabei NO 2 . Dieses wird mit einem Luminoldetektor nachgewiesen. Der Detektor wird alle 2 Stunden kalibriert. Die Kettenlänge wird durch eine Kalibrierung des Gerätes mit HO 2 Radikalen bestimmt, die durch die Photolyse von H 2 O gebildet werden. Der Verstärkungsfaktor wurde in Bezug auf eine Querempfindlichkeit gegen Wasserdampf korrigiert. Die Messgenauigkeit ist etwa 70% bei 60% relativer Feuchte. Messungen am Taunus Observatorium auf dem Kleinen Feldberg in den Sommermonaten der beiden Jahre 1998 und 1999 werden vorgestellt. Die Ozon und RO x Konzentrationen sind gut miteinander korreliert. Allerdings ist die Tagestemperatur die für die Ozon und RO x Konzentrationen bei weitem wichtigste Einflussgröße und ist daher der beste Parameter zur statistischen Beschreibung von photochemischen Vorgängen. Auf der Grundlage der Messungen am Kleinen Feldberg wurde ein einfaches statistisches Modell zur Vorhersage des Ozonmaximums erstellt. Mit den Parametern Temperatur und Ozonkonzentration am Vortag konnte das statistische Modell bereits 80% der Variation der Ozonkonzentration erklären. Durch die Berücksichtigung der RO x Messungen am Vormittag konnte lediglich eine Verbesserung der erklärten Varianz um 0.5% erzielt werden. Um einen Hinweis auf den Einfluss anthropogener Emissionen zu bekommen, wurde der Wochengang von Ozon, RO x und NO x ebenfalls untersucht. Die Zunahme des Ozonmischungsverhältnisses am Wochenende bei gleichzeitigem Rückgang des Mischungsverhältnisses der Stickoxide wird damit erklärt, dass am Kleinen Feldberg eine VOClimitierte Situation vorgefunden wurde. Die Ozonbildungsrate auf Basis der Reaktion zwischen RO x und NO wurde für Tage mit einem Maximum der Globalstrahlung über 600 W m tdatensatz niedrig (r = 0,46). Die beobachtete Änderung des Ozonmischungsverhältnisses wurde mit dem berechneten mittleren Tagesgang der Ozonbildungsrate verglichen. Die Ozonbildungsrate lag um die Mittagszeit bei etwa 5 ppbv h Verlustprozesse zu erklären. Am Abend werden etwa 2 ppbv O 3 pro Stunde abgebaut. Im Rahmen einer Messkampagne im Juni/Juli 2000 am Meteorologischen Observatorium Hohenpeißenberg fanden Messungen der Konzentrationen von RO x , OH, einer Reihe von VOCs, und anderen relevanten Spurengasen statt. Die Messdaten werden mit Hilfe eines auf der Annahme des lokalen photostationären Gleichgewichts der Radikale basierenden Modells interpretiert. Die Modellergebnisse stimmten sehr gut mit den Messungen überein. Die Überschätzung der Konzentration an 2 Tagen wurde durch den Einfluss sauerstoffhaltiger VOCs erklärt. Das '' Recycling" der HO 2 Radikale (die Reaktion zwischen HO 2 und NO) ist die wichtigste Quelle für OH und die wichtigste Senke für RO x . Durch die erhöhte NOKonzentration am Vormittag wird HO 2 sehr schnell in OH umgewandelt, das wiederum für die VOCOxidation und RO x Bildung verantwortlich ist. Die wichtigste OHSenke und RO x Quelle ist die Oxidation von Isopren und den Terpenen. Um die Rolle der photochemischen Ozonbildung auf regionaler Skala zu untersuchen, wurden Ozonmessungen aus ganz Deutschland auf unterschiedlichen zeitlichen und räumlichen Skalen statistisch untersucht. Die Netto Änderungsrate der Ozonkonzentration war tagsüber an 3 nahe zusammenliegenden Stationen sehr ähnlich. Die OzonMessdaten von 277 deutschen Messstationen wurden mit den an einer Waldmessstelle nahe Königstein gemessenen Ozonwerten korreliert. Die Ozonmessungen in Königstein erklären 50% der Varianz der sommerlichen Ozonmessungen zwischen 11:00 und 16:00 MEZ an Stationen, die in einem Umkreis von etwa 250 km von Königstein liegen. Auf das ganze Jahr bezogen, liegt diese ''charakteristische Entfernung" bei etwa 350 km. Diese Ergebnisse deuten darauf hin, dass die Prozesse, die einen wichtigen Einfluss auf die Ozonkonzentration ausüben, auf regionalen Skalen von einigen hundert Kilometern aktiv sind. Zusammenfassend lässt sich sagen, dass die gemessenen RO x Konzentrationen mit den aufgrund der Oxidation der VOCs durch OH berechneten Konzentrationen konsistent sind. Obwohl die RO x Konzentationen für die chemische Modellierung von Bedeutung sind, tragen RO x Messungen nur wenig zu einer Verbesserung der Qualität von kurzfristigen statistischen Ozonprognosen bei. Keywords: Ozone, Troposphere, Peroxy Radicals, Free Radicals, Photochemistry, Chemical Amplifier