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Kontinuierliche Bestimmung von N2O Isotopomeren in Umgebungsluft mittels Quantenkaskadenlaser-Absorptionspektrometrie

English title Continuous N2O isotopomer analysis at ambient concentrations using quantum cascade laser absorption spectrometry
Applicant Emmenegger Lukas
Number 125336
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 01.11.2009 - 31.10.2011
Approved amount 255'269.00
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Keywords (5)

N2O; stable isotopes; quantum cascade laser; spectrometry; spectroscopy

Lay Summary (English)

Lead
Lay summary
Nitrous oxide (N2O) is a stratospheric ozone depleting substance and one of the four most important greenhouse gases. Its major sink, stratospheric destruction, is well quantified, but the global budget is rather uncertain due to a limited understanding of the dominant N2O sources. The study of the three main stable isotopes (14N15N16O / 15N14N16O / 14N14N16O) is a powerful way to trace the biogeochemical cycle of N2O.Absorption spectroscopy in the mid-infrared is potentially the most powerful, direct method to distinguish between all relevant N2O isotopes because of their characteristic rotational-vibrational transitions. It allows the determination of both the N2O concentration and the isotope ratios (?15N? and ?15N?). However, up to now isotope measurements with the required precision of < 1 ‰ for ?15N were only possible at N2O concentration levels that are too high for environmental or atmospheric applications.Based on our latest improvements in laser spectroscopy, we expect a precision for ?15N of 0.1 ‰ at 90 ppm of N2O in a compact and field-deployable quantum cascade laser isotope spectrometer (QCL-IS). While this is adequate to study many biological and technical processes, we also intend to develop a liquid nitrogen-free, fully-automated preconcentration unit. This unit will then be coupled to the QCL-IS to allow continuous ambient air measurements (~320 ppb N2O) with a time resolution of 15 minutes.Studies based on the concentration of individual N2O isotopes and their ratio could significantly enhance our understanding of the global N2O budget. The key to this is source characterization, allocation and quantification of important processes, e.g. soil nitrification/denitrification, waste water treatment and combustion, which will become more accessible because of the novel analytical tool. Furthermore, the preconcentration unit and its coupling to QCLAS is a technique with a wide potential, since it might be used for other trace gases or isotopes with concentrations that are too low for currently available spectroscopy.
Direct link to Lay Summary Last update: 21.02.2013

Responsible applicant and co-applicants

Employees

Name Institute

Publications

Publication
Site selective real-time measurements of atmospheric N2O isotopomers by laser spectroscopy
Mohn Joachim, Tuzson Béla, Manninen Albert, Yoshida Naohiro, Brand Willi A., Emmenegger Lukas (2012), Site selective real-time measurements of atmospheric N2O isotopomers by laser spectroscopy, in Atmospheric Measurement Techniques, 5, 1601-1609.
A liquid nitrogen-free preconcentration unit for measurements of ambient N
Mohn J., Guggenheim C., Tuzson B., Vollmer M.K., Toyoda S., Yoshida N., Emmenegger L. (2010), A liquid nitrogen-free preconcentration unit for measurements of ambient N, in Atmospheric Measurement Techniques, 3, 609-618.

Collaboration

Group / person Country
Types of collaboration
Alpes Lasers SA Switzerland (Europe)
- Industry/business/other use-inspired collaboration
Institute of Plant Nutrition and Soil Science, Christian-Albrechts-University Kiel Germany (Europe)
- in-depth/constructive exchanges on approaches, methods or results
- Publication
- Research Infrastructure
- Exchange of personnel
Rothamsted Research, North Wyke, Okehampton Great Britain and Northern Ireland (Europe)
- in-depth/constructive exchanges on approaches, methods or results
- Research Infrastructure
Department of Crop Science, Section of Plant Nutrition and Crop Physiology, University of Goettingen Germany (Europe)
- in-depth/constructive exchanges on approaches, methods or results
- Publication
- Research Infrastructure
Max Plank Institut, Jena Germany (Europe)
- in-depth/constructive exchanges on approaches, methods or results
- Publication
- Research Infrastructure
Tokyo Institute of Technology Japan (Asia)
- in-depth/constructive exchanges on approaches, methods or results
- Publication
- Research Infrastructure
WSL Switzerland (Europe)
- in-depth/constructive exchanges on approaches, methods or results
- Publication
Institute of Agricultural Climate Research, von Thünen-Institut, Braunschweig Germany (Europe)
- in-depth/constructive exchanges on approaches, methods or results
- Publication
- Research Infrastructure
EAWAG Switzerland (Europe)
- in-depth/constructive exchanges on approaches, methods or results
- Publication
- Research Infrastructure
- Exchange of personnel
ETHZ Switzerland (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
Non-CO2 Greenhouse Gases (NCGG-6) Science, Policy and Integration Talk given at a conference QCLAS in environmental research 31.10.2011 Amsterdam, NL, Netherlands Tuzson Béla; Manninen Albert; Mohn Joachim; Emmenegger Lukas;
Annual Meeting of the German Association for Stable Isotope Research 2011 (GASIR) Talk given at a conference N2O isotopologues by QCLAS 10.10.2011 Villigen, CH, Switzerland Manninen Albert; Emmenegger Lukas; Mohn Joachim;
FLAIR 2011 - Field Laser Applications in Industry and Research Talk given at a conference Frontiers of QCLAS in Isotope Ratio Measurements 13.09.2011 Murnau, D, Italy Tuzson Béla; Emmenegger Lukas;
8th International Conference on Tunable Diode Laser Spectroscopy Talk given at a conference High-precision QCLAS for N2O isotopic species 11.07.2011 Zermatt, CH, Switzerland Tuzson Béla; Manninen Albert; Emmenegger Lukas;
Advances in N tracer experiments and 15N methods Talk given at a conference Development and Field Application of QCLAS for N2O Isotope Ratio Measurements 09.05.2011 Gothenburg, S, Sweden Emmenegger Lukas; Tuzson Béla; Mohn Joachim;
European Geosciences Union General Assembly Talk given at a conference QC laser spectroscopy in environmental monitoring 03.04.2011 Wien, D, Austria Emmenegger Lukas; Tuzson Béla; Manninen Albert; Mohn Joachim;
European Geosciences Union General Assembly 2010 Talk given at a conference Frontiers of stable isotope measurements by QCLAS 02.05.2010 Vienna, D, Austria Manninen Albert; Mohn Joachim; Tuzson Béla;
SIMSUG 2010 Talk given at a conference QCLAS for isotopic ratio measurements 29.04.2010 Exeter, GB, Great Britain and Northern Ireland Emmenegger Lukas; Mohn Joachim; Tuzson Béla;
Stable Isotopes and Biogeochemical Cycles in Terrestrial Ecosystems Talk given at a conference MIR laser spectroscopy for isotopic ratio measurements 21.03.2010 Ascona, CH, Switzerland Mohn Joachim; Manninen Albert; Emmenegger Lukas;
Nitrogen and the European Greenhouse Gas Balance Talk given at a conference Stable isotope measurements of GHG by QCLAS 03.02.2010 Solothurn, CH, Switzerland Emmenegger Lukas; Tuzson Béla; Mohn Joachim;


Self-organised

Title Date Place

Associated projects

Number Title Start Funding scheme
126816 Saisonale und räumliche Charakteriseriung von CO2 Quellregionen basierend auf kontinuierlichen Messungen stabiler CO2 Isotopen mittels Laserspektroskopie am Jungfraujoch 01.05.2011 Project funding (Div. I-III)
150237 N2O from the Swiss midlands - regional sources and hot spots 01.06.2014 Project funding (Div. I-III)
121297 Beschaffung eines Spektrometers basierend auf kontinuierlichen raumtemperatur Quantenkaskadenlasern (CW-RT-QCL) zur Spurengasanalytik 01.01.2009 R'EQUIP
134611 Entwicklung eines Quantenkaskadenlaser Spektrometers zur kontinuierlichen Bestimmung von Methan Isotopen 01.01.2012 Project funding (Div. I-III)
163075 Assessment of the global N2O budget based on seasonal and long-term isotope measurements at Jungfraujoch and the Cape Grim Air Archive 01.12.2016 Project funding (Div. I-III)

Abstract

Nitrous oxide (N2O) is a stratospheric ozone depleting substance and one of the four most important greenhouse gases. Its major sink, stratospheric destruction, is well quantified, but the global budget is rather uncertain due to a limited understanding of the dominant N2O sources. The study of the three main stable isotopes (14N15N16O / 15N14N16O / 14N14N16O) is a powerful way to trace the biogeochemical cycle of N2O. However, isotope-ratio mass-spectrometry (IRMS), the standard analytical tool for stable isotope ratios in trace gases, is generally a laboratory-based instrument and relies on discrete (flask) sampling which limits temporal and spatial resolution capabilities. Additionally, isotopomers such as 14N15N16O and 15N14N16O have the same mass and their quantification by IRMS is therefore a very challenging task, feasible by only a few laboratories.Absorption spectroscopy in the mid-infrared is a direct method to distinguish between all relevant N2O isotopes because of their characteristic rotational-vibrational transitions. It allows the determination of both the N2O concentration and the site specific isotope ratios (d15Na and d15Nb). However, up to now isotope measurements with the required precision of < 1 ‰ for d15N were only possible at N2O concentration levels that are too high for environmental or atmospheric applications. It was only in a recent feasibility study that we obtained a precision of 0.5 ‰ at concentrations of 90 ppm N2O, illustrating that major improvements are possible with mid-infrared quantum cascade laser absorption spectroscopy (QCLAS).In this follow-up project we project a precision for d15N of 0.1 ‰ at 10 ppm of N2O in a compact and field-deployable quantum cascade laser isotope spectrometer (QCL-IS) employing a continuous wave 4.6 müm QCL and a spectral ratio method. While this is adequate to study many biological and technical processes, we also intend to develop a liquid nitrogen-free, fully-automated preconcentration unit. This unit will then be coupled to the QCL-IS to allow continuous ambient air measurements (~320 ppb N2O) with a time resolution of 5 minutes. Finally, this project includes an exemplary field campaign to distinguish N2O source processes based on the site-specific isotopic composition of atmospheric N2O.The work is planned for a two-year study based on one full postdoc position, advised by the experts of our Laboratory for Air Pollution & Environmental Technology with long-term experience on spectroscopy, preconcentration traps and ambient air monitoring.
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