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Invalidation of the Intracavity Optogalvanic Method for Radiocarbon Detection

Published online by Cambridge University Press:  09 February 2016

Cantwell G Carson ,
Martin Stute ,
Yinghuang Ji ,
Roseline Polle ,
Arthur Reboul  and
Klaus S Lackner
Cantwell G Carson
Affiliation:
Earth and Environmental Engineering Department, Columbia University, New York, New York, USA. National Energy Technology Laboratory, U.S. Dept. of Energy, Pittsburgh, Pennsylvania, USA.
Martin Stute
Affiliation:
Department of Environmental Science, Barnard College, New York, New York, USA.
Yinghuang Ji
Affiliation:
Earth and Environmental Engineering Department, Columbia University, New York, New York, USA.
Roseline Polle
Affiliation:
École Polytechnique, Palaiseau, Île-de-France, France. Imperial College London, London, UK.
Arthur Reboul
Affiliation:
École Polytechnique, Palaiseau, Île-de-France, France. Neoen, Paris, Île-de-France, France.
Klaus S Lackner
Affiliation:
Earth and Environmental Engineering Department, Columbia University, New York, New York, USA. The Center for Negative Carbon Emissions, Arizona State University, Tempe, Arizona, USA.
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Abstract

The intracavity optogalvanic spectroscopy (ICOGS) method has been reported to quantify radiocarbon at subambient levels (<1 part per trillion). ICOGS uses a gas sample that is ionized in a low-pressure glow discharge located inside a 14CO2 laser cavity to detect changes in the discharge current under periodic modulation of the laser power to determine the 14CO2 concentration of the sample. When claims of detection thresholds below ambient levels were not verified by other researchers, we constructed a theoretical analysis to resolve differences between these conflicting reports and built and tested an ICOGS system to establish a lower limit of detection. Using a linear absorbance model of the background contribution of 12CO2 and data from the HITRAN database, we estimate that the limit of detection (3σx) is close to 1.5×104 Modern. By measuring a 1.5×104 Modern enriched CO2 sample in a cavity modulation ICOGS system without a clear signal, we conclude that for this system the limit of detection for ICOGS must be above 1.5×104. The implications for previous ICOGS reports are discussed.

Keywords

Intracavity optogalvanic spectroscopy (ICOGS)radiocarbonlaser spectroscopymonitoring verification and accounting
Type
Research Article
Information
Radiocarbon , Volume 58 , Supplement 1 , March 2016 , pp. 213 - 225
Copyright
© 2016 by the Arizona Board of Regents on behalf of the University of Arizona 

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