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Entwicklung eines Quantenkaskadenlaser Spektrometers zur kontinuierlichen Bestimmung von Methan Isotopen

English title Development of a real-time quantum cascade laser spectrometer for methane isotopic species in ambient air
Applicant Emmenegger Lukas
Number 134611
Funding scheme Project funding (Div. I-III)
Research institution Luftfremdstoffe / Umwelttechnik 500 - Mobility, Energy and Environment EMPA
Institution of higher education Swiss Federal Laboratories for Materials Science and Technology - EMPA
Main discipline Climatology. Atmospherical Chemistry, Aeronomy
Start/End 01.01.2012 - 31.12.2015
Approved amount 253'236.00
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All Disciplines (2)

Discipline
Climatology. Atmospherical Chemistry, Aeronomy
Other disciplines of Physics

Keywords (4)

Laser spectroscopy; Trace gases; Methane isotopes; Quantum cascade laser

Lay Summary (English)

Lead
Lay summary

influences the abundance of ozone and the concentration of hydroxyl radicals which impacts virtually all of atmospheric chemistry.4 in promoting global warming. Furthermore, CH2) is the second most important of the anthropogenically influenced greenhouse gases. On a per-molecule basis it is 25 times more effective than CO4Methane (CH

The total global methane emissions are relatively well known but the strength of each source component and their trends are not. Since the major source categories and the OH sink have distinct isotopic signatures in d13 and 4C-CHd4D-CH, high-frequency and high-precision measurements of these parameters would help constraining emission sources and the global budget. However, isotope-ratio mass-spectrometry (IRMS), the standard analytical tool for stable isotope ratios in trace gases, is a laboratory-based technique which limits temporal and spatial resolution capabilities.

Alternatively, a isotopic species because of their characteristic rotational-vibrational transitions. 4bsorption spectroscopy in the mid-infrared is a direct method to distinguish between all relevant CHD, and the respective isotope ratios 3 and CH4CH13, 4CH12Within this project we will thus develop an instrument to continuously monitor d13 and 4C-CHd4D-CH, using state of the art quantum cascade laser absorption spectrometry (QCLAS). The instrument will be based on recently developed 7.5 µm, continuous wave room temperature lasers (cw-RT-QCL) and a novel astigmatic multipath cell with an optical path length of 200 m. To obtain the necessary precision of 0.1‰ (d13) and 14C-CH‰ (d4D-CH), the QCLAS will be coupled to an automated, liquid-nitrogen free preconcentration unit.

Direct link to Lay Summary Last update: 21.02.2013

Responsible applicant and co-applicants

Employees

Name Institute

Publications

Publication
Real-time analysis of d13C- and dD-CH4 in ambient air with laser spectroscopy: method development and first intercomparison results
Eyer Simon, Tuzson Bela, Popa M. Elena, van der Veen Carina, Röckmann Thomas, Rothe Michael, Brand Willi A., Fisher Rebecca, Lowry Dave, Nisbet Euan G., Brennwald Matthias S., Harris Eliza, Zellweger Christoph, Emmenegger Lukas, Fischer Hubertus, Mohn Joachim (2016), Real-time analysis of d13C- and dD-CH4 in ambient air with laser spectroscopy: method development and first intercomparison results, in Atmospheric Measurement Techniques, 9, 263-280.
Methane preconcentration by adsorption: a methodology for materials and conditions selection
Eyer Simon, Tuzson Bela, Stadie Nicolas, Borgschulte Andreas, Emmenegger Lukas, Mohn Joachim (2014), Methane preconcentration by adsorption: a methodology for materials and conditions selection, in Adsorption, 20(5-6), 657-666.
In-situ observations of the isotopic composition of methane at the Cabauw tall tower site
Röckmann Thomas, Eyer Simon (shared first author), van der Veen Carina, Popa M. Elena, Tuzson Bela, Monteil Guillaume, Houweling Sander, Harris Eliza, Brunner Dominik, Fischer Hubertus, Zazzeri Giulia, Lowry Dave, Nisbet Euan G., Brand Willi A., Necki Jaroslaw M., Emmenegger Lukas, Mohn Joachim, In-situ observations of the isotopic composition of methane at the Cabauw tall tower site, in Atmospheric Chemistry and Physics Discussions.

Collaboration

Group / person Country
Types of collaboration
Prof. N. Buchmann / ETHZ Switzerland (Europe)
- in-depth/constructive exchanges on approaches, methods or results
- Exchange of personnel
Dr. Willi A. Brand / MPI Jena Germany (Europe)
- in-depth/constructive exchanges on approaches, methods or results
- Research Infrastructure
Aerodyne Research / Center for Atmospheric and Environmental Chemistry United States of America (North America)
- in-depth/constructive exchanges on approaches, methods or results
- Research Infrastructure
Prof. Thomas Röckmann / Utrecht University Netherlands (Europe)
- in-depth/constructive exchanges on approaches, methods or results
- Publication
- Research Infrastructure
- Exchange of personnel
Inst. for quantum electronics / ETHZ Switzerland (Europe)
- in-depth/constructive exchanges on approaches, methods or results
- Exchange of personnel
Prof. Hubertus Fischer / Uni Bern Switzerland (Europe)
- in-depth/constructive exchanges on approaches, methods or results
- Research Infrastructure
Prof. Euan Nisbet / RHUL Great Britain and Northern Ireland (Europe)
- in-depth/constructive exchanges on approaches, methods or results
- Publication

Scientific events

Active participation

Title Type of contribution Title of article or contribution Date Place Persons involved
INGOS EU FP7 Final Conference Talk given at a conference Real-time analysis of d13C- and dD-CH4 in ambient air with laser spectroscopy: Method development and intercomparison 23.09.2015 Utrecht, Netherlands Eyer Simon; Fischer Hubertus; Emmenegger Lukas; Tuzson Béla;
International Symposium on Non-CO2 Greenhouse Gases (NCGG7) Talk given at a conference On-site analysis of d13C- and dD-CH4 by laser spectroscopy for the allocation of source processes 07.11.2014 Amsterdam, Netherlands Tuzson Béla; Eyer Simon; Fischer Hubertus; Emmenegger Lukas;
General Assembly European Geoscience Union (EGU) Talk given at a conference Real-time analysis of d13C- and dD-CH4 by high precision laser spectroscopy 02.04.2014 Vienna, Austria Eyer Simon; Tuzson Béla; Fischer Hubertus; Emmenegger Lukas;
INGOS EU FP7 Workshop Talk given at a conference Development of a real-time quantum cascade laser spectrometer for methane isotopic species in ambient air 28.10.2013 Bern, Switzerland Eyer Simon; Fischer Hubertus; Emmenegger Lukas; Tuzson Béla;
ASI 2013 Talk given at a conference A real-time quantum cascade laser spectrometer for methane isotopic spiecies in ambient air 30.09.2013 Braunschweig, Germany Fischer Hubertus; Emmenegger Lukas; Tuzson Béla; Eyer Simon;
SIBAE Workshop Talk given at a conference Recent Advances in Laser Spectroscopic Analysis of GHG Stable Isotopes 14.05.2013 Wrzlav, Poland Tuzson Béla; Eyer Simon; Emmenegger Lukas;
INGOS EU FP7 Workshop Talk given at a conference Development of a real-time quantum cascade laser spectrometer for methane isotopic species in ambient air 12.03.2013 Bremen, Germany Tuzson Béla; Emmenegger Lukas; Fischer Hubertus; Eyer Simon;
AIRMONTEC FP7 Workshop Talk given at a conference Multi-component laser spectroscopy: on the way to the all-in-one laser sensor 04.03.2013 Duisburg, Germany Tuzson Béla; Emmenegger Lukas;
Swiss Chemical Society Fall Meeting Talk given at a conference Optimization of CH4 adsorption from ambient air for high precision isotopic analysis 13.09.2012 Zürich, Switzerland Fischer Hubertus; Emmenegger Lukas; Eyer Simon; Tuzson Béla;
JESIUM2012 Talk given at a conference Optimization of CH4 adsorption from ambient air for high precision isotopic analysis 03.09.2012 Leipzig, Germany Eyer Simon; Emmenegger Lukas; Tuzson Béla;
Laser Optics Talk given at a conference Application of direct absorption mid IR laser spectroscopy for isotope specific detection of greenhouse gases 25.06.2012 St. Petersburg, Switzerland Tuzson Béla; Eyer Simon; Emmenegger Lukas;


Knowledge transfer events

Active participation

Title Type of contribution Date Place Persons involved
Natural Resources and Pollutant NAREP Seminar (talk: Real-time analysis of d13C- and dD-CH4 in ambient air with laser spectroscopy: Method development and first applications) Talk 07.12.2015 Dübendorf, Switzerland Tuzson Béla; Emmenegger Lukas; Eyer Simon; Fischer Hubertus;
Naturforschende Gesellschaft Oberwallis (talk: Neue Methoden zur Erforschung des Treibhausgases Methan) Talk 20.05.2015 Brig, Switzerland Emmenegger Lukas; Fischer Hubertus; Tuzson Béla; Eyer Simon;
Technical Meeting on Stable Isotope Reference Materials (talk: Use of optical isotope analyzers for GHG, namely N2O, CO2, and CH4 and instrument calibration strategies) Talk 01.09.2014 Vienna, Austria Emmenegger Lukas; Tuzson Béla;


Communication with the public

Communication Title Media Place Year
Talks/events/exhibitions Neue Methoden zur Erforschung des Treibhausgases Methan Western Switzerland 2015

Awards

Title Year
ACP Award for Atmospheric Research, granted by the Atmospheric Chemistry and Physics Commission (ACP) of the Swiss Academy of Sciences (sc|nat+). 2016
Award for the best oral presentation of a young scientist, ASI 2013, Braunschweig 2013

Associated projects

Number Title Start Funding scheme
150237 N2O from the Swiss midlands - regional sources and hot spots 01.06.2014 Project funding (Div. I-III)
172585 N2O from the Swiss midlands - regional sources and hot spots - 18 month extension 01.06.2017 Project funding (Div. I-III)
125336 Kontinuierliche Bestimmung von N2O Isotopomeren in Umgebungsluft mittels Quantenkaskadenlaser-Absorptionspektrometrie 01.11.2009 Project funding (Div. I-III)

Abstract

The total global methane source is relatively well known but the strength of each source component and their trends are not. Since the major source categories and the OH sink have distinct isotopic signatures in d13C-CH4 and dD-CH4, high-frequency and high-precision measurements of the these parameters would improve the constrains for emission sources and the global budget. However, isotope-ratio mass-spectrometry (IRMS), the standard analytical tool for stable isotope ratios in trace gases, is generally a laboratory-based technique which limits temporal and spatial resolution capabilities.Alternatively, absorption spectroscopy in the mid-infrared is a direct method to distinguish between all relevant CH4 isotopic species because of their characteristic rotational-vibrational transitions. Within this project we will thus develop an instrument to continuously monitor 12CH4, 13CH4 and CH3D, and the respective isotope rations d13C-CH4 and dD-CH4, based on state of the art quantum cascade laser absorption spectrometry (QCLAS). The instrument will be based on recently developed 7.5 µm, continuous wave room temperature lasers (cw-RT-QCL) and a novel astigmatic multipath cell with an optical path length of 200 m. To obtain the necessary precision of 0.1‰ (d13C-CH4) and 1‰ (dD-CH4), the QCLAS will be coupled to an automated, liquid-nitrogen free preconcentration unit. Validation will include the careful evaluation of fractionation effects, methan concentration dependence, as well as direct comparison with state of the art IRMS.The project is based on the work of one PhD student and the strong competence in laser spectroscopy, trace gas monitoring and IRMS of the involved research partners.
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