High-precision laser spectrometer for multiple greenhouse gas analysis in 1 mL air from ice core samples

Bereiter, Bernhard; Tuzson, Béla; Scheidegger, Philipp; Kupferschmid, André; Looser, Herbert; Mächler, Lars; Baggenstos, Daniel; Schmitt, Jochen; Fischer, Hubertus; Emmenegger, Lukas (2020). High-precision laser spectrometer for multiple greenhouse gas analysis in 1 mL air from ice core samples. Atmospheric Measurement Techniques, 13(11), pp. 6391-6406. Copernicus Publications 10.5194/amt-13-6391-2020

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The record of past greenhouse gas composition from ice cores is crucial for our understanding of global climate change. Future ice core projects will aim to extend both the temporal coverage (extending the timescale to 1.5 Myr) and the temporal resolution of existing records. This implies a strongly limited sample availability, increasing demands on analytical accuracy and precision, and the need to reuse air samples extracted from ice cores for multiple gas analyses. To meet these requirements, we designed and developed a new analytical system that combines direct absorption laser spectroscopy in the mid-infrared (mid-IR) with a quantitative sublimation extraction method. Here, we focus on a high-precision dual-laser spectrometer for the simultaneous measurement of CH4, N2O, and CO2 concentrations, as well as d13C(CO2). Flow-through experiments at 5 mbar gas pressure demonstrate an analytical precision (1 sigma) of 0.006 ppm for CO2, 0.02‰ for d13C(CO2), 0.4 ppb for CH4, and 0.1 ppb for N2O, obtained after an integration time of 100 s. Sample–standard repeatabilities (1 sigma) of discrete samples of 1 mL STP (Standard Temperature and Pressure) amount to 0.03 ppm, 2.2 ppb, 1 ppb, and 0.04‰ for CO2, CH4, N2O, and d13C(CO2), respectively. The key elements to achieve this performance are a custom-developed multipass absorption cell, custom-made high-performance data acquisition and laser driving electronics, and a robust calibration approach involving multiple reference gases. The assessment of the spectrometer capabilities in repeated measurement cycles of discrete air samples – mimicking the procedure for external samples such as air samples from ice cores – was found to fully meet our performance criteria for future ice core analysis. Finally, this non-consumptive method allows the reuse of the precious gas samples for further analysis, which creates new opportunities in ice core science.

Item Type:

Journal Article (Original Article)

Division/Institute:

08 Faculty of Science > Physics Institute > Climate and Environmental Physics
10 Strategic Research Centers > Oeschger Centre for Climate Change Research (OCCR)
08 Faculty of Science > Physics Institute

UniBE Contributor:

Bereiter, Bernhard; Mächler, Lars; Baggenstos, Daniel; Schmitt, Jochen and Fischer, Hubertus

Subjects:

500 Science > 530 Physics

ISSN:

1867-8548

Publisher:

Copernicus Publications

Funders:

[18] European Research Council

Projects:

[UNSPECIFIED] deepSLice (grant agreement no. 667507)

Language:

English

Submitter:

Hubertus Fischer

Date Deposited:

03 Dec 2020 15:02

Last Modified:

03 Dec 2020 15:02

Publisher DOI:

10.5194/amt-13-6391-2020

BORIS DOI:

10.7892/boris.148603

URI:

https://boris.unibe.ch/id/eprint/148603

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