Airborne in situ measurements of short-lived chlorocarbons and investigation of their pathways from northern hemispheric source regions into the lowermost [...] / von Valentin Michael Lauther. Wuppertal, 2020
Content
Abstract
Introduction
Transport into the lowermost stratosphere
Tracer-tracer correlation
Overview on CH2Cl2 and CHCl3
Sources of CH2Cl2 and CHCl3
Global source regions of CH2Cl2 and CHCl3
Sinks and lifetime
Impact on ozone
Aircraft measurements of CH2Cl2 and CHCl3
Outline of this thesis
HAGAR-V hardware development and characterization
The instrument and its measurement principle
Preconcentration unit
Preconcentration unit design
Temperature measurement for the preconcentration trap
Temperature characterization for the preconcentration trap
Breakthrough volumes for different adsorbents
Memory effects
Fast gas chromatography
Linearity of signal response
First operation on the HALO research aircraft
Analysis and processing of WISE MS data
WISE (Wave-driven ISentropic Exchange)
Peak fitting
Calculation of HAGAR-V MS mixing ratios for WISE data
Detrending
Calibration methods
Correction of jumps in the detector response
Systematic bias of in-flight SPAN measurements
System contamination during WISE
Influence of inlet pumps
Comparison with other instruments
Investigation of transport of CH2Cl2 and CHCl3 into the UTLS
Chemical Lagrangian Model of the Stratosphere
The CH2Cl2-N2O correlation
Correlation branch filter
Background mixing ratios of CH2Cl2
Impact of different source regions
Seasonal dominance of regional sources
Trajectory transport times and source regions
Major updraft events
Transport pathways
The CHCl3-N2O correlation
Background mixing ratios of CHCl3
Impact of different source regions
Comparison of CHCl3 and CH2Cl2
Impact of hurricane Maria
CH2Cl2 and CHCl3 measurements around major population centers in East Asia
Summary
Synopsis and outlook
Detailed description of HAGAR-V
HAG_01 - Power Distribution Box
HAG_02 - Base module and HAG_07 - Display
HAG_03 - Gas Supply
HAG_04 - ECD
HAG_05 - MS/Licor
HAG_06 - Power / cRIO
MS module characterizations
Breakthrough volumes
BTV of the preconcentration trap used during WISE
BTV preconcentration trap with Graphsphere 2017
BTV of a multi adsorbent preconcentration trap
Memory effects
Measurement setup of test for signal linearity
Limit of detection (LOD)
HAGAR-V during the aircraft campaign WISE
Pre-flight preparations
Issues during WISE
Overheating
Dehydrating of air samples
Regulation of mass flow controller
Very strong adsorbent
Species that were not usable for scientific analysis
MS module parameters during WISE
MS module: data processing
Approximation of the EMG fit
Analysis of systematic bias of in-flight SPAN measurements
Peak height vs peak area
Analysis of system contamination during WISE
Analysis of SPAN-to-pump measurements
Detailed comparison with other instruments
Calibrations and relative accuracy
Calibration of primary working standard
Calibration of in-flight calibration gases
WISE MS relative accuracy estimates
Supplemental information about the CH2Cl2-N2O correlation
Supplemental information about measurement locations
Supplemental graphs of emission tracers
Supplemental statistics about the correlation branch filter
Supplemental information about the CHCl3-N2O correlation
The positions of measurement
Supplemental information about emission tracers
Seasonal dominance of source regions for CHCl3
Supplemental information about measurements associated with hurricane Maria
Supplemental information about backward trajectories
Supplemental information about MIRAH and EMeRGE–Asia samples
Nomenclature
List of Figures
List of Tables
Bibliography
Acknowledgments