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Temperature Dependent Absorption Cross-Sections of O3 and NO2

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Temperature Dependent Absorption Cross-Sections of O3 and NO2 ” Temperature Dependent Absorption Cross-Sections of O3 and NO2 in the 240 - 790 nm range determined by using the GOME-2 Satellite Spectrometers for use in Remote Sensing Applications” Dissertation zur Erlangung des akademischen Grades eines Doktors der Naturwissenschaften (Dr. rer. nat.) am Fachbereich Physik der Universit¨at Bremen vorgelegt von Dipl.-Physiker Bilgehan G¨ur Bremen, Februar 2006 1. Gutachter: Prof. Dr. rer. nat. John P. Burrows 2. Gutachter: Dr. rer. nat. habil. Johannes Orphal Eingereicht am: 21.02.2006 Tag des Promotionskolloquims: 05.05.2006 Abstract Absorption spectra of O3 and NO2 have been measured in three independent campaigns using the three highly stabilized and accurately characterized GOME-2 satellite spec- trometers, flight models FM2, FM2-1, and FM3. GOME-2 (Global Ozone Monitoring Experiment) is an enhanced follow-up project of GOME, which was launched on ESA’s second European Remote Sensing Satellite (ERS-2) in 1995. A new generation of satellites for earth observation will be available with the MetOp se- ries, starting most likely in the second half of 2006. MetOp comprises three polar-orbiting satellites to be launched sequentially over 14 years. One of the operational instruments onboard these satellites will be GOME-2, a nadir-viewing spectrometer that observes so- lar radiation transmitted or scattered from the Earth atmosphere or from its surface. Spectra were recorded at five temperatures (203 K, 223 K, 243 K, 273 K, and 293 K) for O3 and four temperatures (223 K, 243 K, 273 K and 293 K) for NO2 with a spectral coverage of 240 to 790 nm at a resolution of 0.24 to 0.53 nm full width at half maximum. The relative temperature dependences were determined. The achieved set of laboratory measurements of O3 absorption spectra is in very good agreement (about 1-3 % at 293 K) with the recommended O3 absorption cross sections at 10 different wavelengths. For the temperature dependence in the range of 400 to 450 nm an upper limit estimate of no more than 10 % decrease with falling temperature was found at 425 to 430 nm in disagreement with one previous publication. There is some evidence that continuous absorption as measured in the blue wing of the Chappuis band at 429.5 nm drops by a few percent when temperature is reduced from 293 K to 203 K. At the same time the peak of the band at 426.5 nm increases slightly by 1 %. This is supported by a clear increase of amplitude of differential absorption cross≈ section at 426 nm of 13 % with falling temperature. At 604.61nm at the top of the Chappuis band a slight increase of cross section with falling temperature of 1 % is found in agreement with three previous publications and in disagreement with on≈e most recent one. The measurements of NO2 absorption spectra are in very good agreement with literature data and recommended NO2 absorption cross sections at ambient temperature (about 1-2 % in the main DOAS window between 400 and 500 nm). The determined temperature dependence is in agreement with previous observations, i.e. a linear increase of the peak- to-valley absorbance difference with decreasing temperature from 293 K to 223 K. The purpose of this study is mainly focused on the clarification of the above mentioned open issues regarding the O3 absorption cross sections. Nevertheless both sets of newly achieved absorption spectra of O3 and NO2 are of high importance as reference data for remote sensing, and will be used to derive (with GOME-2) a detailed picture of the atmospheric content and profile of O3, NO2 and other trace gases. It will furthermore help to validate and improve the spectroscopic database. Contents 1 Introduction and Motivation 5 2 Atmospheric Chemistry 13 2.1 TheEarth’sAtmosphere ............................ 13 2.2 StratosphericChemistry . 16 2.2.1 O3 in the Global Stratosphere and the Role of NO2 ......... 16 2.2.2 Ozone Depletion in the Polar Regions . 18 2.2.3 Ozone Depletion in Mid Latitudes . 20 2.3 TroposphericChemistry ............................ 21 2.3.1 O3 and NO2 intheTroposphere . 21 3 Relevant Aspects of Molecular Spectroscopy 23 3.1 MolecularSpectroscopy. 23 3.1.1 ElectronicSpectra ........................... 26 3.1.2 VibrationalSpectra. 28 3.1.3 RotationalSpectra ........................... 29 3.1.4 Symmetry Properties of Polyatomic Molecules . ..... 32 3.2 Absorption-Spectrum of O3 .......................... 35 3.3 Absorption-Spectrum of NO2 ......................... 40 4 Experimental Setup 41 4.1 TheGOME-2Spectrometer . 41 4.2 TheCATGASSetup .............................. 44 4.2.1 Light-Sourceandoptics . 45 4.2.2 Gas-Vessel................................ 46 4.2.3 Gas-System O3 ............................. 46 4.2.4 Gas-System NO2 ............................ 51 4.3 TheOpticalInterface. 58 5 Data-Aquisition 61 5.1 Measurement-ProcedurewithGOME-2 . 61 5.1.1 Documentation of measured Intensities I0 and I ........... 62 5.2 Reference-Interpolation and Calculation of Optical Densities . 66 5.3 ConcatenationofaSpectrum . 68 5.3.1 Quality analysis of overlap region . 72 3 5.4 Origin-Projects ................................. 73 5.4.1 Data................................... 73 5.4.2 Spectra ................................. 75 5.4.3 Baselines................................. 78 6 Wavelength Calibration 79 7 O3-Absorption Measurements with GOME-2 83 7.1 Integrated Absorption Cross Sections . 84 7.2 Absolute Scaling of the GOME-2 O3-Spectra................. 87 7.2.1 Final GOME-2 O3-Spectra ...................... 92 7.3 Results and Comparison with Literature Data Base . 96 7.3.1 Comparison of GOME-2 spectra at ambient temperature with lit- erature values at 10 single wavelengths . 97 7.3.2 Comparison of relative temperature dependence . ..... 99 7.3.3 Modelling the temperature dependence of O3 by a polynomial fit . 106 7.3.4 Comparison of available spectra in the Huggins bands . 108 7.3.5 Integrated cross sections at different temperatures . .......112 7.4 ErrorAnalysisandPropagation . 115 8 NO2-Absorption Measurements with GOME-2 119 8.1 Correction of the N2O4-Absorption ......................120 8.2 Absolute Scaling of the NO2 Spectra obtained from GOME-2 Measurements122 8.2.1 Final GOME-2 NO2-Spectra......................122 8.3 Results and Comparison with Literature Data Base . 124 8.3.1 Comparison of GOME-2 data with literature at ambient temperature124 8.3.2 Temperature dependence of NO2 spectra obtained from the GOME- 2study .................................130 9 Outlook 135 10 Conclusion 137 A Quality-Analysis Overlap Region 139 B I0 - I Documentation 145 Chapter 1 Introduction and Motivation Although minor constituents, ozone (O3) and nitrogen dioxide (NO2) are central species in atmospheric processes and therefore of major interest in research activities. O3 had already been discovered in 1840 by C.F. Sch¨onbein, who suggested the presence of an atmospheric gas having a peculiar odor. He called this gas ”ozone”, coming from ”ozein”, the Greek word for scent and smell. Since then, many studies have been performed to describe different aspects of ozone, such as molecular properties, the chemical basis of its existence in the atmosphere and its interaction with other atmospheric components. Spectroscopic studies showed already in the late 19th century that ozone is present at higher concentrations in the upper atmospheric layers than close to the ground, leading to the term ”ozone layer”. Nowadays it is not only in the scientific community well known that this layer is of high importance for human life on earth because of one decisive optical property of ozone, i.e. its absorption of biologically harmful ultra violet radiation. In the 1970’s a research group from the British Antarctic Survey, who was moni- toring the atmosphere above Antarctica, noticed a dramatic loss of ozone in the lower stratosphere over Antarctica. It is reported that when the first measurements were taken in 1985, the drop in ozone levels in the stratosphere was so dramatic that at first the scientists thought their instru- ments were faulty. Replacement instruments were built and flown out, and it wasn’t until they confirmed the earlier measurements, several months later, that the ozone depletion observed was accepted as genuine. Satellite measurements were becoming available at the same time and showed indeed also a massive depletion of ozone on a large scale over most of the Antarctica continent (figure 1.1). However, these were initially rejected as unreasonable by data quality control algorithms (they were filtered out as errors since the values were unexpectedly low); the ozone hole was only detected in satellite data when the raw data was reprocessed following evidence of an ozone hole in the above mentioned in situ observations. From thereon the ozone hole attracted worldwide publicity and caused increased re- search activities. 5 6 CHAPTER 1. INTRODUCTION AND MOTIVATION A further atmospheric trace gas of importance is nitrogen dioxide NO2. Nitrogen ox- ides (NOx) in general are emitted by combustion processes and play a key part in the catalytic production of tropospheric ozone by photochemical processes. This affects the local air quality as well as the global tropospheric chemistry. NO2 can therefore be used as an indicator for air pollution. Here as well satellite based observations provide such information on a global scale. Just recently Richter et al. [1]published results from mea- surements with the satellite instruments GOME (Global Ozone Monitoring Experiment) and SCIAMACHY (Scanning Imaging Absorption Spectrometer for Atmospheric CHar- tographY), indicating an increase of tropospheric NO2 over China and showing also air polluted regions over Europe (figures 1.2 and 1.3). Figure 1.1: Ozone depletion at 1980 and 1991 over the south pole, recorded with the satel- lite instrument TOMS (Total Ozone Mapping Spectrometer) [With friendly permission from the Center for Atmospheric Sciences at the University of Cambride]. 7 VC NO2 [molec / cm 2 ] > 4.0 x 1016 2.0 x 1016 16 e 1.0 x 10 d u t i t 15 a 5.0 x 10 L 2.0 x 1015 1.0 x 1015 5.0 x 1014 Longitude Figure 1.2: Tropospheric column amounts of NO2 over China retrieved from the satellite instruments GOME and SCIAMACHY [1].
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