Main text The pilot study CCQM-P204 was aimed at evaluating the level of compatibility of laboratories' measurement capabilities to value assign isotope ratios in samples of pure CO 2 gas, expressed as isotope delta values relative to the relevant international scale: δ 13 C VPDB and δ 18 O VPDB-CO2 . Pure CO 2 gas samples were prepared by the BIPM in batches of 10 samples of the same gas and circulated to participants for measurement. Each participant received four samples of CO 2 with a different nominal δ 13 C VPDB value: −1 ‰; −9 ‰; −35 ‰; and −42 ‰. The BIPM was also responsible for evaluating the homogeneity and stability of the samples. The co-coordinator IAEA received one sample per batch to confirm the batch-to-batch homogeneity. Within-batch and between-batch inhomogeneity was assessed and found to be negligible in comparison to the spread of results reported by participants. Participants used the analytical technique of their choice to measure the isotope delta values. They were requested to report the measurement results together with detailed information on their traceability, measurement methods and data treatment. Results of the comparison were to be compiled by the BIPM and evaluated jointly by the BIPM and the IAEA. The majority of participants reported results using DI-IRMS, and those that reported results based on laser spectroscopy techniques showed a very similar dispersion of results as for DI-IRMS, although generally with greater uncertainty. A total of nineteen participants reported their measurements, with two of them reporting results with different reference materials to provide more insight into the traceability of the measurements. The results were reported with traceability to three different VPDB scale realizations, notably VPDB, VPDB-LSVEC and VPDB2020, with 8, 7 and 6 results reported respectively for each of these. Participants agreed that results based on VPDB and VPDB2020 scale realizations should, in principle, lead to consistent results, whereas those based on VPDB-LSVEC should show a bias that increased as samples became more depleted in 13 C, with the bias approaching 0.2 ‰ for the most depleted sample. This bias was demonstrated by the participant reporting the most precise measurements based on the VPDB-LSVEC realizations, whereas for 2 participants using VPDB-LSVEC scale realizations other issues dominated the consistency of their results. The 3 laboratories using the NIST (8562,8563, 8564) reference materials (reported as on the VPDB-LSVEC scale), were highly consistent with each other, but the reported bias for the VPDB-LSVEC realization was not evident, with the historical method used for value assignment of the NIST RMs, and their relatively large uncertainty, being identified as possible causes for this. In general, for all results the dispersion was greater than expected based on the measurement uncertainties reported by participants. This dispersion increased as the samples became more depleted in 13 C, so that results that were traceable to realizations of the VPDB scale that could be considered equivalent (VPDB and VPDB2020) did not lead to ensembles that were fully consistent within their stated uncertainties. Either the reduced chi-squared or Birge Ratio provide easily calculated quantities to characterise lack of consistency in a data set, where consistent data would lead to values of unity for either of these, and discrepant data leading to increased values. This is most readily demonstrated by considering results based on DI-IRMS with traceability to the VPDB scale through either VPDB and VPDB 2020 realizations, where the standard deviation of 16 results was 0.043 ‰ and a Birge Ratio of 2.7 calculated for nominally −1‰ for δ 13 C, and the standard deviation was 0.12 ‰ and a Birge Ratio of 2.9 calculated at nominally −9 ‰ for δ 18 O. For the samples where the nominal δ 13 C value was −42 ‰, the standard deviation of 17 results was 0.085 ‰ and a Birge Ratio of 4.5 calculated for δ 13 C, and the standard deviation was 0.24 ‰ and a Birge Ratio of 3.4 calculated for δ 18 O at nominally −36 ‰. The observed magnitude of the standard deviation of results can also be compared to the standard uncertainty of the IAEA-603 materials certified values (0.01 ‰ for δ 13 C and 0.04 ‰ δ 18 O) and the smallest standard uncertainties reported by a participant (0.005 ‰ for δ 13 C, and 0.01 ‰ for δ 18 O). These results indicate an underestimation of uncertainty for reported results, especially for those with the smallest uncertainties. Components of uncertainty that should be reviewed before future comparisons include: the uncertainty contribution from reference materials; the uncertainty associated with the phosphoric acid reaction with carbonate reference materials; corrections and uncertainties related to cross-contamination effects in the IRMS; appropriate methods for combining uncertainties of multiple reference materials and accounting for their correlations. A retreatment of results, which normalizes results to the −1 ‰ and −42 ‰ δ 13 C samples, leads to improvement in the consistency of results as demonstrated for measurements on the nominally −35 ‰ δ 13 C, −30 ‰ δ18O samples for which the standard deviation is reduced to 0.034 ‰ and 0.057 ‰ for δ 13 C and δ 18 O respectively (from 0.072 ‰ and 0.198 ‰ without normalization). The results of the comparison indicate that once issues of non-ideal methods and use of LSVEC are removed, discrepancies in results arise from the challenges in accurately transferring delta values from carbonate reference materials to CO 2 gaseous samples, and that these issues can be reduced by having appropriate gaseous reference standards for calibration when measuring CO 2 gaseous samples. This is consistent with the identical treatment principle that is preferred in the isotope ratio measurement community. An analysis of results is presented in this report, with further consideration of the impact of the measurement method, the scale, and the reference materials. Uncertainties reported by participants are detailed and analysed, highlighting important differences in the uncertainty sources considered. Although CCQM-P204 was a comparison organised within the CCQM/GAWG and IRWG, no reference value was calculated, mainly because not all results appeared to be strictly on the same scale. Instead, a list of recommendations is provided to encourage more harmonised measurement practices and reach better consistency in future comparisons on similar materials. To reach the main text of this paper, click on Final Report . Note that this text is that which appears in Appendix B of the BIPM key comparison database https://www.bipm.org/kcdb/ . The final report has been peer-reviewed and approved for publication by the CCQM, according to the provisions of the CIPM Mutual Recognition Arrangement (CIPM MRA).

Main text This pilot study evaluates the coherence of carbon isotope delta reference materials (RMs) used by laboratories worldwide. The goal was to assess how well laboratories can realize the VPDB scale using these RMs. In total, carbon isotope delta values of 36 RMs were measured by seven laboratories as well as the vanillin sample previously evaluated in CCQM-K167/P211. A hierarchical Bayesian measurement model was used to evaluate the coherence between these RMs, and to determine the carbon isotope delta value of each of these RMs. In general, this study shows that the 36 carbon isotope delta RMs are reliable. Further, the value assigned to the vanillin sample in this study is within 0.02 ‰ from the CCQM-K167 KCRV. To reach the main text of this paper, click on Final Report . Note that this text is that which appears in Appendix B of the BIPM key comparison database https://www.bipm.org/kcdb/ . The final report has been peer-reviewed and approved for publication by the CCQM, according to the provisions of the CIPM Mutual Recognition Arrangement (CIPM MRA).

With global warming and increasing water use, tap water resources need sustainable management. We used hydrogen and oxygen isotope analyses in tap water (i.e.,δ2H andδ18O values) to identify issues associated with tap water resources in Canada. We analyzed 576 summer tap samples collected from across Canada and 76 tap samples from three cities during different seasons and years. We classified the samples based on their sources: groundwater (TapGroundwater), river (TapRiver) and lake (TapLake).δ2H values in tap water correlate strongly with values predicted for local precipitation across Canada with a stronger correlation for TapGroundwaterand TapRiverthan for TapLake.We then constructed water balance models to predict theδ2H of surface water across Canada, and validated them against Canadian streamδ2H data.δ2H values in tap water correlate strongly with values predicted for local surface water, however, the water balance models improved the predictability only for TapRiverand TapLakeand not for TapGroundwater. TapGroundwaterδ2H values reflect theδ2H values of annually averaged precipitation, whereas TapRiverand TapLakeδ2H values reflect post-precipitation processes. We used theδ2H residuals between the observed and predictedδ2H values to assess regional processes influencing tap waterδ2H values across Canada. Regionally, snow/glacier melt contributes to all tap sources around the Rockies. Tap waters are highly evaporated across Western Canada, irrespective of their sources. In the Great Lakes and East Coast regions, tap waters are evaporated in many localities, particularly those using surface reservoirs and lakes. We propose the use of these isotopic baselines as a way forward for the monitoring of tap water resources at different scales. These isotopic baselines also have valuable applications in human forensic studies in Canada.

Main text This pilot study was conducted in parallel to the key comparison CCQM-K167. Vials containing 0.25 mg of vanillin were prepared at NRC and distributed to four participating institutes. Institutes could choose any suitable reference materials and methodology to perform carbon isotope delta measurements. Participants reported analysis details, and a carbon isotope delta value and associated uncertainty for the vanillin sample. Each of the carbon isotope delta results of vanillin were compared to the KCRV established from CCQM-K167, and metrological compatibility to the KCRV was determined. Three expert laboratories participated in this study, and their reported results serve as a benchmark to compare the performance of all other participants to these world-class institutes. To reach the main text of this paper, click on Final Report. The final report has been peer-reviewed and approved for publication by the CCQM.

Stable carbon isotope ratio measurements are used to investigate the provenance of vanillin. In this study, a variety of commercial vanillin samples and vanilla products were analyzed to provide a frame of reference for the variability of carbon isotope delta values in various vanillin samples, with the results ranging from −20.6 to −36.7‰ relative to the Vienna Peedee Belemnite (VPDB). We present information on the development of two synthetic vanillin reference materials, VANA-1 and VANB-1, prepared in 0.75 g units in glass vials, to be used for the calibration of carbon isotope delta measurements of vanillin and other easily combustible organic materials. Characterization of 40 vials each of VANA-1 and VANB-1 was performed by three laboratories over several measurement sequences. The certified carbon isotope delta values are −31.30 ± 0.06‰ (VANA-1) and −25.85 ± 0.05‰ (VANB-1). These uncertainties, for the 95

Main text The CCQM Isotope Ratio Working Group (IRWG) determined that an additional key comparison of carbon isotope delta measurements was required to capture the progress of this field. Vials containing 0.25 mg of vanillin were prepared at NRC, and evaluated for bottle-to-bottle homogeneity prior to distribution to the eight participating institutes. Participants were able to choose any suitable method and reference materials for carbon isotope delta measurements, and report a carbon isotope delta value and the associated uncertainty, and analysis details. To determine the key comparison reference value (KCRV) and its associated uncertainty, the NRC in collaboration with the NIST, developed a multivariate Bayesian random laboratory effects model, which also incorporates the uncertainty due to bottle-to-bottle homogeneity and any correlations between the reported results that arise due to the use of common reference materials. The KCRV for this study was determined to be -25.833 ‰ relative to the VPDB, with associated uncertainty of 0.028 ‰, and expanded uncertainty of 0.056 ‰ (k=2). All the results reported by the participants in this study were considered equivalent to the KCRV. To reach the main text of this paper, click on Final Report. Note that this text is that which appears in Appendix B of the BIPM key comparison database https://www.bipm.org/kcdb/. The final report has been peer-reviewed and approved for publication by the CCQM, according to the provisions of the CIPM Mutual Recognition Arrangement (CIPM MRA).

Here, we review the contributions of Professor Barbara Sherwood Lollar to Compound Specific Isotope Analysis (CSIA) in contaminant hydrogeology and environmental chemistry. We first discuss the seminal work by Professor Sherwood Lollar's lab on establishing CSIA as a quantitative tool for contaminant (bio)transformation at contaminated groundwater sites. We describe the critical research by her lab in the development and validation of sample collection techniques, single- and multi-element CSIA, and isotope data evaluation for reliable interpretations. We highlight the contributions of Professor Sherwood Lollar's lab towards the development of best practices for the successful application of CSIA by industry to demonstrate the occurrence of (bio)transformation, identify (bio)transformation mechanisms, quantify the extent and rate of degradation and differentiate among potential contaminant sources. We then explore Professor Sherwood Lollar's applications of CSIA to hydrogeology of the deep subsurface and the fast widening of the field to new environments (e.g., sediments), contaminants (e.g., chlorofluorocarbons, pesticides), and systems (e.g., plant, enzymes).

Vanillin, one of the world’s most popular flavor used in food and pharmaceutical industries, is extracted from vanilla beans or obtained (bio)-synthetically. The price of natural vanillin is considerably higher than that of its synthetic alternative which leads increasingly to counterfeit vanillin. Here, we describe the workflow of combining carbon isotope ratio combustion mass spectrometry with quantitative carbon nuclear magnetic resonance spectrometry (13C-qNMR) to obtain carbon isotope measurements traceable to the Vienna Peedee Belemnite (VPDB) with 0.7‰ combined standard uncertainty (or expanded uncertainty of 1.4‰ at 95% confidence level). We perform these measurements on qualified Bruker 400 MHz instruments to certify site-specific carbon isotope delta values in two vanillin materials, VANA-1 and VANB-1, believed to be the first intramolecular isotopic certified reference material (CRMs).

Abstract Stable hydrogen, carbon, nitrogen, oxygen and sulfur (HCNOS) isotope compositions expressed as isotope-delta values are typically reported relative to international standards such as Vienna Standard Mean Ocean Water (VSMOW), Vienna Peedee belemnite (VPDB) or Vienna Cañon Diablo Troilite (VCDT). These international standards are chosen by convention and the calibration methods used to realise them in practice undergo occasional changes. To ensure longevity and reusability of published data, a comprehensive description of (1) analytical procedure, (2) traceability, (3) data processing, and (4) uncertainty evaluation is required. Following earlier International Union of Pure and Applied Chemistry documents on terminology and notations, this paper proposes minimum requirements for publishing HCNOS stable-isotope delta results. Each of the requirements are presented with illustrative examples.

Unidentified human remains have historically been investigated nationally by law enforcement authorities. However, this approach is outdated in a globalized world with rapid transportation means, where humans easily move long distances across borders. Cross-border cooperation in solving cold-cases is rare due to political, administrative or technical challenges. It is fundamental to develop new tools to provide rapid and cost-effective leads for international cooperation. In this work, we demonstrate that isotopic measurements are effective screening tools to help identify cold-cases with potential international ramifications. We first complete existing databases of hydrogen and sulfur isotopes in human hair from residents across North America by compiling or analyzing hair from Canada, the United States (US) and Mexico. Using these databases, we develop maps predicting isotope variations in human hair across North America. We demonstrate that both δ 2 H and δ 34 S values of human hair are highly predictable and display strong spatial patterns. Multi-isotope analysis combined with dual δ 2 H and δ 34 S geographic probability maps provide evidence for international travel in two case studies. In the first, we demonstrate that multi-isotope analysis in bulk hair of deceased border crossers found in the US, close to the Mexico-US border, help trace their last place of residence or travel back to specific regions of Mexico. These findings were validated by the subsequent identification of these individuals through the Pima County Office of the Medical Examiner in Tucson, Arizona. In the second case study, we demonstrate that sequential multi-isotope analysis along the hair strands of an unidentified individual found in Canada provides detailed insights into the international mobility of this individual during the last year of life. In both cases, isotope data provide strong leads towards international travel.

Human remains, later named "Madame Victoria", were discovered in 2001 near the Royal Victoria hospital in Montreal but were never identified by forensic practitioners. We use multi-isotope hair profiles to investigate Madame Victoria's travel and diet history. Based on carbon isotope abundances, Madame Victoria had a stable diet and values typical of eastern Canada. Nitrogen isotope ratios are more positive than average Canadians, and increase sharply over the last two months of her life, likely reflecting a rapid health deterioration. Hydrogen isotope abundances are typical of eastern Canada, and become stepwise more positive throughout the hair profile. Based on hydrogen isotope data, Madame Victoria moved progressively from either a western Ontario or northern Quebec locality towards Montreal over the last 3 years of her life stopping multiple times along the way. The strontium isotope ratios are constant throughout the hair profile and equal to the isotopic value of the soil exchangeable strontium at the site where the body was discovered. This observation, combined with hair major and trace elemental data, indicates that strontium from soil diffused and replaced the original hair strontium post-mortem. This study shows the interest of multi-isotope hair profiles to focus investigations on cold cases but also underlines the need for further work to take advantage of metal and metal isotope data.

By convention, carbon isotope ratios are expressed relative to VPDB defined by the calcite standard NBS19 in the 1980s. [See T. Coplen, Pure Appl. Chem. 1994, 66, 273-276.] To improve the realization of the VPDB scale, a second fixed point (lithium carbonate, LSVEC) was introduced in 2006 [T. Coplen et al. Anal. Chem. 2006, 78, 2439-2441], which is now known to be isotopically unstable. [Assonov, S. Rapid Commun. Mass Spectrom., 2018, 32, 827-830.] With the high-quality reference materials made available in 2020, it is now possible to realize the VPDB scale with high confidence. [Assonov, S. et al. Rapid Commun. Mass Spectrom., 2020, 34, e8867; Assonov, S. Rapid Commun. Mass Spectrom. 2021, 35, e9014; Qi, H. et al. Rapid Commun. Mass Spectrosc. 2021, 35, e9006.] Here, we report the analysis of 25 reference materials using isotope ratio combustion mass spectrometry, show the discontinuity between the values measured against the new IAEA reference materials and the values currently assigned to these reference materials on the VPDB2006, and provide a link bringing these materials onto the new VPDB2020.

Studying the isotope variability in fast-growing human tissues (e.g., hair, nails) is a powerful tool to investigate human nutrition. However, interpreting the controls of this isotopic variability at the population scale is often challenging as multiple factors can superimpose on the isotopic signals of a current population. Here, we analyse carbon, nitrogen, and sulphur isotopes in hair from 590 Canadian resident volunteers along with demographics, dietary and geographic information about each participant. We use a series of machine-learning regressions to demonstrate that the isotopic values in Canadian residents' hair are not only influenced by dietary choices but by geographic controls. First, we show that isotopic values in Canadian residents' hair have a limited range of variability consistent with the homogenization of Canadian dietary habits (as in other industrialized countries). As expected, some of the isotopic variability within the population correlates with recorded individual dietary choices. More interestingly, some regional spatial patterns emerge from carbon and sulphur isotope variations. The high carbon isotope composition of the hair of eastern Canadians relative to that of western Canadians correlates with the dominance of corn in the eastern Canadian food-industry. The gradient of sulphur isotope composition in Canadian hair from coast to inland regions correlates with the increasing soil pH and decreasing deposition of marine-derived sulphate aerosols in local food systems. We conclude that part of the isotopic variability found in the hair of Canadian residents reflects the isotopic signature associated with specific environmental conditions and agricultural practices of regional food systems transmitted to humans through the high consumption rate of intra-provincial food in Canada. Our study also underscores the strong potential of sulphur isotopes as tracers of human and food provenance.

Forensic practitioners, archeologists, and ecologists increasingly use hair isotope profiles and isotope databases and maps to reconstruct the life history of unidentified individuals. Relationships between hair isotope profiles with travel history have been primarily investigated through controlled laboratory experiments. However, those controlled studies do not reflect the complex life history of modern individuals who often travel between multiple locations over different periods. Here, we collect one bundle of hairs from a volunteer whose primary residence is in Ottawa (Canada) but who traveled to multiple destinations over a period of 18 months. Those travels include multi-week trips to distant locations and multi-day trips to more local areas. We use multi-isotope profiles on the individual’s hairs coupled with isotope databases across the world to reconstruct travel history at sub-monthly temporal resolution. We compare the isotopic interpretation of mobility with the recorded travel history. A prominent shift in δ2H values is interpreted as a westward movement toward central Canada, which corresponds to a month-long road-trip to the Prairie. We observed a marked negative excursion in δ13C values along the hairs profile, which was related to a multi-week-long trip to several countries in Europe. Except for an exceptionally variable interval likely driven by health issues, δ15N values show very little fluctuation across the entire profile, indicating consumption of consistent amounts of animal or marine-based protein at different locations. The isotopic shifts in the proximal part of the hair reveal a clearer picture of traveling destinations than the shifts in the distal part, which have larger uncertainty in terms of timing and amplitude. Except for the last couple of months before collection, 87Sr/86Sr ratios show little variation throughout the profile likely due to recent exchange with Ottawa tap water during bathing or showering. The different 87Sr/86Sr ratios in the month preceding collection appear to partially preserve the 87Sr/86Sr ratio of the volunteer’s diet. This study demonstrates the interest of using multi-isotope systems and large isotopic databases to reconstruct individual mobility. This study also underlines the challenges in linking isotope data to mobility, particularly in rapidly growing keratinous tissues.

Stable carbon isotope (δ(13C)) analysis can provide information concerning the starting materials and the production process of a material. Carbon nanotubes (CNTs) are produced using a variety of starting materials, catalysts, and production methods. The use of δ(13C) as a tool to infer the nature of starting materials to gain insight into the mechanics of CNT growth was evaluated. The production process of NRC's SWCNT-1 was traced via the δ(13C) measurement of the available starting materials, intermediate products, and the final product. As isotopic fractionation is likely negligible at high temperatures, the δ(13C) value of the starting materials was reflected in the δ(13C) value of the final CNT product. For commercially available CNTs, the estimated δ(13C) values of identified starting materials were related to the δ(13C) signatures of CNTs. Using this information and the δ(13C) values of CNTs, the nature of unknown carbon sources was inferred for some samples. The use of δ(13C) analysis may be used as a tracer to differentiate between those processes that use relatively 13C-depleted carbon source(s) such as carbon monoxide, methane, or natural gas, and those that do not.

Over 200 sugars, high sugar content foods, and sugar-free alternative products found in Canadian supermarkets were analyzed for carbon isotope (δ13C) values, adding to the record of food items with reported δ13C values, which can aid in food authentication and human diet studies. The δ13C values of the products were mostly consistent with the photosynthetic pathway of the plant from which the main ingredients were derived. With the exception of those sugars and syrups derived from known C3 sources, all of the sugars and syrups and most of the sugar added to food products were from C4 plants such as sugar cane or corn syrup. Many sweeteners are chemically manufactured, and most reflect an intermediate δ13C value. A mixing model estimated the contribution of C3- and C4-based ingredients in foods with high sugar content, which may be used to evaluate the percentage of added sugar from C3- or C4-sources.

RATIONALE:For isotope delta analysis, it is preferable to have at least two matrix-matched reference materials whose isotope delta values encompass those of the samples to be analyzed. The National Research Council Canada (NRC) has developed three sugar Certified Reference Materials (CRMs), BEET-1 (beet sugar), GALT-1 (galactose), and FRUT-1 (fructose), to be collectively used for carbon isotope delta measurements in sugars, and other organic materials. METHODS:All materials were homogenized and packaged in glass ampules. All three sugar materials were analyzed at the NRC using elemental analyzer/isotope ratio mass spectrometry (EA/IRMS). Six additional laboratories also provided EA/IRMS measurements. Data from all laboratories were re-normalized using three international secondary reference materials (IAEA-CH-6, USGS40, and USGS62) included as blind samples in the inter-laboratory comparison, thus providing added quality control and robustness to the study. RESULTS:Re-normalized carbon isotope delta values from each laboratory were combined using a random laboratory effects statistical model with accounting of the correlations between the laboratory results due to the use of the same reference materials for calibration. The consensus δ(13 C) values and combined standard uncertainties which include effects due to characterization, homogeneity, and stability for BEET-1, GALT-1, and FRUT-1 are -26.02(7) ‰, -21.41(6) ‰, and -10.98(5) ‰, respectively, on the VPDB scale. CONCLUSIONS:Three new δ(13 C) sugar CRMs (BEET-1, GALT-1, and FRUT-1) were developed and are available from NRC. These three CRMs can be utilized as a set for daily δ(13 C) scale normalization of sugar-based or other organic materials in order to produce reliable δ(13 C) measurements.

Background: Economically motivated adulteration (EMA) of foods has become an increasing concern in recent years, with lemon juice as a popular target. Objective and Method: In this work, an optimized preparation procedure for the isolation of citric acid from lemon juice was validated using elemental analyzer-isotope ratio MS (EA-IRMS) to detect adulteration with exogenous citric acid. Additionally, 69 imported lemon juice samples were evaluated using combustion module-cavity ring down spectrometry (CM-CRDS) and compared with the well-established EA-IRMS. Equivalency of CM-CRDS to EA-IRMS was further demonstrated by conducting a round-robin study involving eight laboratories throughout the United States, Canada, and New Zealand. Results: Overall, the results obtained for CM-CRDS were statistically indistinguishable from the results obtained using EA-IRMS for EMA lemon juice analysis. Conclusions: Therefore, CM-CRDS is a viable option for this application. Highlights: The CM-CRDS instrumentation is easy to operate, robust, and provides δ13C values comparable to EA-IRMS for citrate analysis. Through a multi-laboratory exercise, CM-CRDS was shown to be an alternative to EA-IRMS in the detection of economic adulteration of lemon juice.

Isotope delta measurements are normalized against international reference standards. Although multi-point normalization is becoming a standard practice, the existing uncertainty evaluation practices are either undocumented or are incomplete. For multi-point normalization, we present errors-in-variables regression models for explicit accounting of the measurement uncertainty of the international standards along with the uncertainty that is attributed to their assigned values. This manuscript presents framework to account for the uncertainty that arises due to a small number of replicate measurements and discusses multi-laboratory data reduction while accounting for inevitable correlations between the laboratories due to the use of identical reference materials for calibration. Both frequentist and Bayesian methods of uncertainty analysis are discussed.

Actinides can be measured by alpha spectroscopy (AS), mass spectroscopy or accelerator mass spectrometry (AMS). We tested a simple method to separate Pu and Am isotopes from the sample matrix using a single extraction chromatography column. The actinides in the column eluent were then measured by AS or AMS using a fluoride target matrix. Pu and Am were coprecipitated with NdF3. The strongest AMS beams of Pu and Am were produced when there was a large excess of fluoride donor atoms in the target and the NdF3 precipitates were diluted about 6–8 fold with PbF2. The measured concentrations of 239,240Pu and 241Am agreed with the concentrations in standards of known activity and with two IAEA certified reference materials. Measurements of 239,240Pu and 241Am made at A.E. Lalonde AMS Laboratory agree, within their statistical uncertainty, with independent measurements made using the IsoTrace AMS system. This work demonstrated that fluoride targets can produce reliable beams of actinide anions and that the measurement of actinides using fluorides agree with published values in certified reference materials.