Airborne and ground level flask sampling for regional carbon budgets [Elektronische Ressource] : the potential of multiple tracer and isotope analyses ; development of a new Investigation Strategy and of an improved Sampling System / vorgelegt von Marcus Schumacher

Informations

• Publié par: universitat_hamburg
• Publié le: 01 janvier 2005
• Nombre de lectures: 15
• Langue: English
• Poids de l'ouvrage: 18 Mo

Extrait

AIRBORNE AND GROUND LEVEL FLASK SAMPLING FOR
REGIONAL CARBON BUDGETS – THE POTENTIAL OF
MULTIPLE TRACER AND ISOTOPE ANALYSES

Development of a new ‘Investigation Strategy’ and of an improved
‘Sampling System’














Dissertation
zur Erlangung des Doktorgrades
der Naturwissenschaften im Fachbereich
Geowissenschaften
der Universität Hamburg








Vorgelegt von
Marcus Schumacher
aus
Gifhorn



Hamburg
2005


Als Dissertation angenommen vom Fachbereich Geowissenschaften der
Universität Hamburg

Auf Grund der Gutachten von Professor Dr. Hartmut Graßl
und Professor Dr. Martin Heimann


Hamburg, den 11. Juli 2005


Professor Dr. H. Schleicher
Dekan des Fachbereichs Geowissenschaften


PREAMBLE

Some of the most important problems and questions focussed on in this thesis
were identified by field experiments performed within a major project initiated and
carried out by several groups.
The investigations, as well as the resulting enhancements presented here are
mainly reactions attributed to campaign observations. Therefore the newly
designed sampling system, the ground reference unit and the sophisticated
investigation strategy have arisen as means to an end – and were not the intended
purposes of this study. To accomplish the findings a particular venture was the
critical scrutiny and the adaptation of established assumptions.

Since the data acquisition was carried out within the restricting frame of the main
project specific experiments were only possible in a limited fashion. More flights
would have been desirable, also because the amount of data obtained from the
field campaigns is low.

As a corollary, the result of this study is not a register with regional carbon
‘numbers’, but a list with aspects and impairments which have to be taken into
account, providing the basis for further investigations focussing on airborne and
ground based assessment of the carbon budget.

In spite of, or thanks to the adverse conditions, new findings and ideas could be
deduced which shall be applied in succeeding projects.





‘And therefore as a stranger give it welcome …’ PREAMBLE
1. INTRODUCTION
2. BASIC PRINCIPLES: THEORY AND EXPERIMENTAL SETUP
2.1. Theory
2.1.1.1. Long lived Trace Gases in the Atmosphere 4
Carbon Dioxide in the Atmosphere 5
Additional Trace Gases 7
2.1.1.2. Isotopic Signatures in Carbon Dioxide 13
2.1.2. RECAB Strategy 19
2.1.3. Convective Boundary Layer 25
2.1.4. Ground Characterization and References 28
2.1.5. Combined Investigations
2.1.5.1. Modelling Approaches – Inverse Studies 29
2.1.5.2. Land Use Classification 31
2.2. System Configurations and Data Analysis
2.2.1. Campaign Equipment
2.2.1.1. Flight Sampling Unit 34
2.2.1.2. Continuous Flight Measurements 35
2.2.1.3. Ground Reference System 36
2.2.2. Equipment Gas Analyses
2.2.2.1. Trace Gas Mixing Ratios from Flask Sampling 38
2.2.2.2. Isotope Ratios 39 3. TEST FLIGHTS AND LABORATORY EXPERIMENTS
3.1. Test Flight Measurements October 2000-May 2001
3.1.1. Description of the German Study Region
3.1.1.1. Geography and Climate 40
3.1.1.2. Field Sites 41
3.1.2. Hainich Flights October 2000 43
3.1.3. Winter Flights January and February 2001 45
3.1.4. Gebesee Flights May 2001 47
3.2. Development of a modified Flask Sampling System
3.2.1. Conventional System:
48 Test of the inlet tubing and of the gas exchange rate
October – December 2000
3.3. Modified Flask Sampling System
3.3.1. Modified System:
Adjustment of the flow rate and tests regarding effects of the drying
51
reagent on the CO mixing ratio 2
September – December 2001
3.3.1.1. Exchange characteristic 51
3.3.1.2. Influence of the drying medium on the CO mixing ratio 52 2
3.3.2. Comparison of the different sampling systems January 2002 54
3.4. Summary of the modifications and assessment of the
57
improvements 4. RECAB FIELD EXPERIMENTS JUNE 2001 – AUGUST 2002
4.1. Data Acquisition and Observations
4.1.1. Valencia Summer Experiment 17 June – 7 July 2001
60
First experiment with the modified sampling system
4.1.2. Thuringia Summer Experiment 15 July – 2 August 2001 62
4.1.3. Uppland Summer Experiment 11 August - 9 September 2001
63
Implementation of additional trace gases analyses
4.1.4. Valencia Winter Experiment 16 November – 15 December 2001
66
Final configuration of the modified sampling system
4.1.5. The Netherlands Winter Experiment 14 January – 10 February 2002
69
Test of improved sampling strategy
4.1.5. Lazio Summer Experiment 27 May – 27 June 2002 73
4.1.7. The Netherlands Summer Experiment 10 – 28 July 2002
75
Enhancement of improved sampling strategy
134.1.8. ‘SPA CE’ Thuringia Summer Experiment 6 – 15 August 2002
77
Combined ground level and flight investigations
4.2. Interpretation of the Results
Southern Europe
4.2.1. Valencia Summer Experiment 80
4.2.2. Valencia Winter Experiment 81
4.2.3.1. Lazio Summer Experiment 84
4.2.3.2. Inverse Study - Mesoscale Dispersion Model 86
4.2.3.3. Inverse Study - Back Trajectory Calculations 88
Northern Europe
4.2.4. Uppland Summer Experiment 90 Central Europe
4.2.5. Thuringia Summer Experiment 94
4.2.6. The Netherlands Winter Experiment 95
4.2.7. The Netherlands Summer Experiment 97
13
4.2.8.1. ‘SPA CE’ Thuringia Summer Experiment 102
4.2.8.2. Inverse Study - Adjoint of a Transport Model 108
5. DISCUSSION
5.1. Comparison of the Study Regions using Multiple Tracer Data
13
5.1.1. CO / delta C and CO / CO relationships 2 2
Carbon Dioxide and Isotopic Signature 111
Combustion Processes 113
5.1.2. Comparison of the study regions
5.1.2.1. Seasonal Variations 115
5.1.2.2. Longitudinal Differences 119
5.1.2.3. Latitudinal Differences 122
5.2. Theoretical and Conceptual Aspects
5.2.1. Time Dependence 127
Variability - Air Mass Change 129
Day-to-day Variability 130
Local Characteristics – Land-Sea-Wind Circulation 132
‘Signal Shift’ – Effects of time delayed Detection 133
CH and VOC Conversion 4 135
5.2.2. Applicability of the ‘CBL-budget Approach’ 141 5.3. Summary of Methodological Experiences 143
Identified Impairments 145
5.4. Enhanced Investigation Strategy
5.4.1. Implementation of Ground Reference Measurements and Sampling 148
5.4.2. Adapted Flight Investigation Strategy – ‘Transect Approach’ 151
6. CONCLUSIONS
6.1. Relevance of the Results 155
6.2. Perspectives 156
158 7. SUMMARY
8. ANNEXES
A1 ABBREVIATIONS and CONVERSION OF UNITS 161
A2 EQUIPMENT Configuration of Sampling Units 162
A3 EQUIPMENT Configuration of Analytical Instrumentation 163
A4 EQUIPMENT Instrument Manufacturers 164
A5 Laboratory Experiment January 2002 166
A6 Scale Basis for Triplet Calculations 168
A7 Trace gas mixing ratios and isotopic composition of CO from the 2
169 RECAB field campaigns for the lowest flight level and for the free
troposphere
9. REFERENCES 170
198 10. ACKNOWLEDGEMENTS 1. INTRODUCTION

As soon as mankind appeared on the scene some hundred thousand years ago it
formed its environment. But during the last few hundred years the human impact
became more and more distinct, because of the broadening and intensification
which came along with the growth of population and the increase of the living
standards and economic demands.
These anthropogenic interferences are influencing not only the terrestrial surface
but also the atmosphere. Effects, which became apparent during the last two
decades, are for example the ozone hole, the acid rain and the summer smog
phenomena, and more recently the ‘addi