Ever since the first publication of intracavity optogalvanic spectroscopy (ICOGS) in 2008, this novel technique for measuring the (14)C/(12)C ratio in carbon dioxide has rendered considerable attention. As a result, there are currently at least five different research groups pursuing research on ICOGS. With a claimed limit of detection of 10(-15) ((14)C/(12)C), i.e., in the same order as accelerator mass spectroscopy, achieved with a relatively inexpensive and uncomplicated table-top system, ICOGS has major scientific and commercial implications. However, during the past 5 years, no research group has been able to reproduce these results or present additional proof for ICOGS's capability of unambiguous (14)C detection, including the authors of the original publication. Starting in 2010, our group has set up a state-of-the-art ICOGS laboratory and has investigated the basic methodology of ICOGS in general and tried to reproduce the reported experiments in particular. We have not been able to reproduce the reported results concerning the optogalvanic signals dependence on (14)C concentration and wavelength and, ultimately, not seen any evidence of the capability of ICOGS to unambiguously detect (14)C at all. Instead, we have found indications that the reported results can be products of measurement uncertainties and mistakes. Furthermore, our results strongly indicate that the reported limit of detection is likely to be overestimated by at least 2 orders of magnitude, based on the results presented in the original publication. Hence, we conclude that the original reports on ICOGS cannot be confirmed and therefore must be in error.
Accelerator mass spectrometry (AMS) is by far the predominant technology deployed for radiocarbon tracer studies. Applications are widespread from archaeology to biological, environmental, and pharmaceutical sciences. In spite of its excellent performance, AMS is expensive and complicated to operate. Consequently, alternative detection techniques for 14 C are of great interest, with the vision of a compact, user-friendly, and inexpensive analytical method. Here, we report on the use of intracavity optogalvanic spectroscopy (ICOGS) for measurements of the 14 C/ 12 C ratio. This new detection technique was developed by Murnick et al. (2008). In the infrared (IR) region, CO 2 molecules have strong absorption coefficients. The IR-absorption lines are narrow in line width and shifted for different carbon isotopes. These properties can potentially be exploited to detect 14 CO 2 , 13 CO 2 , or 12 CO 2 molecules unambiguously. In ICOGS, the sample is in the form of CO 2 gas, eliminating the graphitization step that h is required in most AMS labs. The status of the ICOGS setup in Uppsala is presented. The system is operational but not yet fully developed. Data are presented for initial results that illustrate the dependence of the optogalvanic signal on various parameters, such as background and plasma-induced changes in the sample gas composition.