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Dissertation Universität Bremen Fachbereich 1 - Physik Institut Für Umweltphysik Dissertation Universität Bremen Fachbereich 1 - Physik Institut für Umweltphysik Studies on the Transport of CO and Related Biomass Burning Emissions Using Ground-based Fourier Transform Infrared Spectrometry Vorgelegt von Voltaire Velazco zur Erlangung des Grades Doktor rerum naturalium (Dr. rer. nat) 1. Gutachter: Prof. Dr. Justus Notholt 2. Gutachter: Prof. Dr. Klaus Künzi April 2006 TABLE OF CONTENTS ABSTRACT ................................................................................................................................... 3 ZUSSAMMENFASSUNG .................................................................................................................. 4 LIST OF PUBLICATIONS WITHIN THE LAST THREE YEARS ............................................................ 5 1. INTRODUCTION..................................................................................................................... 6 1.1. C OMPOSITION OF THE EARTH ’S ATMOSPHERE ....................................................................... 7 1.2. L AYERS OF THE ATMOSPHERE .............................................................................................. 8 2. INSTRUMENTATION .......................................................................................................... 10 2.1. T HE FOURIER TRANSFORM INFRARED (FTIR) S PECTROMETER .......................................... 10 2.2. A DDITIONAL FEATURES AND ADVANTAGES OF A FOURIER TRANSFORM INFRARED (FTIR)12 SPECTROMETER ......................................................................................................................... 12 3. RETRIEVAL THEORY ........................................................................................................ 14 3.1. I NTRODUCTION TO SOLVING INVERSE PROBLEMS ............................................................... 14 3.1.1. The least Squares Solution to an Inverse Problem ..................................................... 14 3.1.2. Estimating the Errors of the Solution ......................................................................... 15 3.1.3. Resolution Matrix of the Solution ............................................................................... 16 3.1.4. Optimal Estimation ..................................................................................................... 17 3.2. I MPROVEMENTS ON THE RETRIEVAL PROCESS .................................................................... 18 3.2.1. Optimizing the Retrieval Strategy............................................................................... 18 3.2.2. A priori Profile Information of the Target Molecules ................................................ 18 3.2.3. Strategy for Specific Molecules .................................................................................. 21 3.2.3.1. Strategy for CO.................................................................................................... 21 3.2.3.2. CO Averaging Kernels......................................................................................... 21 3.2.3.2. Strategy for C 2H6 ..................................................................................................... 24 3.2.2.3. O 3 Triplet Spectroscopy Applied to C 2H6 Retrievals .......................................... 24 3.2.2.3. O 3 Triplet Spectroscopy Applied to C 2H6 Retrievals .......................................... 25 4. RESULTS AND DISCUSSIONS........................................................................................... 29 4.1. S ENSITIVITY STUDIES ON THE DEPENDENCE OF THE CO RETRIEVALS ON THE A PRIORI INFORMATION ............................................................................................................................ 30 4.1.1. Introduction................................................................................................................. 30 4.1.2. Results......................................................................................................................... 31 4.1.3. Summary ..................................................................................................................... 35 4.2. L ATITUDE AND ALTITUDE VARIABILITY OF CARBON MONOXIDE IN THE ATLANTIC DETECTED FROM SHIP -BORNE FOURIER TRANSFORM SPECTROMETRY , M ODEL AND SATELLITE DATA ......................................................................................................................................... 36 4.2.1. Introduction................................................................................................................. 36 4.2.2. MOPITT data.............................................................................................................. 36 4.2.3. Model data from MATCH-MPIC................................................................................ 37 4.2.4. Five Polarstern Cruises from 1996-2003 ................................................................... 37 4.2.5. FTIR, Model and Satellite Data.................................................................................. 41 4.2.6. Simulating Low- Resolution Retrievals from High Resolution Retrievals.................. 41 4.2.7. Assessment of CO sources .......................................................................................... 43 4.2.8. Summary ..................................................................................................................... 46 4.3. T HE IMPACT OF FOREST FIRES ON CO CONCENTRATIONS IN THE NORTHERN HEMISPHERE 47 1 TABLE OF CONTENTS 4.3.1. Introduction: Fires in the Ecosystem.......................................................................... 47 4.3.2 The El Niño Phenomenon ............................................................................................ 47 4.3.2.1. The El Niño episode in 1997-1998........................................................................... 48 4.3.3 Long Term Measurements of Trace Gases in the Arctic and the effects of Fires in 1998 ............................................................................................................................................... 49 4.3.4. Measurements of CO, C 2H6 and HCN in Spitsbergen ................................................ 52 4.3.5. Summary ..................................................................................................................... 56 4.4. A Q UANTITATIVE ASSESSMENT OF THE 1998 CO A NOMALY IN THE NORTHERN HEMISPHERE BASED ON TOTAL COLUMN MEASUREMENTS WITH FTIR S PECTROMETRY .......... 57 4.4.1. Introduction................................................................................................................. 57 4.4.2. Experimental Techniques............................................................................................ 57 4.4.3. Error Estimates........................................................................................................... 57 4.4.4. Results......................................................................................................................... 59 4.4.5. Quantifying the Effects of the 1998 Anomaly in the Free Troposphere ..................... 60 4.4.6. Summary ..................................................................................................................... 65 4.5. INVESTIGATIONS OF POLAR STRATO -MESOSPHERIC CARBON MONOXIDE MEASURED BY GROUND -BASED FOURIER TRANSFORM INFRARED SPECTROMETRY .......................................... 67 4.5.1. Introduction................................................................................................................. 67 4.5.2. Instruments.................................................................................................................. 68 4.5.3. Retrieval of Strato-Mesospheric CO........................................................................... 68 4.5.4. The Chemical Transport Model.................................................................................. 69 4.5.5 Results.......................................................................................................................... 72 4.5.5.1. FTIR data and model calculations ....................................................................... 72 4.5.5.2. Quantifying the CO above 18 km ........................................................................ 72 4.5.6. Summary ..................................................................................................................... 76 4.6. M EASUREMENTS OF CO AND HCN IN PARAMARIBO , S URINAME ....................................... 77 4.6.1. Introduction................................................................................................................. 77 4.6.2 The Inter-tropical Convergence Zone (ITCZ).............................................................. 78 4.6.3. Results......................................................................................................................... 78 4.6.3.1. Peak in the signal caused by emissions from fires............................................... 78 4.6.3.2. Perturbations detected in the mid to upper troposphere....................................... 78 4.6.3.3. Backward trajectories confirm ITCZ migration .................................................. 79 4.6.5. Effects of the ITCZ migration on the total columns of HCN and CO......................... 79 4.6.6. Summary ....................................................................................................................
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