Carbonate clumped isotope analysis (Δ47 ) of 21 carbonate standards determined via gas-source isotope-ratio mass spectrometry on four instrumental configurations using carbonate-based standardization and multiyear data sets.

RATIONALE: Clumped isotope geochemistry examines the pairing or clumping of heavy isotopes in molecules and provides information about the thermodynamic and kinetic controls on their formation. The first clumped isotope measurements of carbonate minerals were first published 15 years ago, and since then, interlaboratory offsets have been observed, and laboratory and community practices for measurement, data analysis, and instrumentation have evolved. Here we briefly review historical and recent developments for measurements, share Tripati Lab practices for four different instrument configurations, test a recently published proposal for carbonate-based standardization on multiple instruments using multi-year data sets, and report values for 21 different carbonate standards that allow for recalculations of previously published data sets. METHODS: We examine data from 4628 standard measurements on Thermo MAT 253 and Nu Perspective IS mass spectrometers, using a common acid bath (90°C) and small-sample (70°C) individual reaction vessels. Each configuration was investigated by treating some standards as anchors (working standards) and the remainder as unknowns (consistency standards). RESULTS: We show that different acid digestion systems and mass spectrometer models yield indistinguishable results when instrument drift is well characterized. For linearity correction, mixed gas-and-carbonate standardization or carbonate-only standardization yields similar results. No difference is observed in the use of three or eight working standards for the construction of transfer functions. CONCLUSIONS: We show that all configurations yield similar results if instrument drift is robustly characterized and validate a recent proposal for carbonate-based standardization using large multiyear data sets. Δ47 values are reported for 21 carbonate standards on both the absolute reference frame (ARF; also refered to as the Carbon Dioxide Equilibrated Scale or CDES) and the new InterCarb-Carbon Dioxide Equilibrium Scale (I-CDES) reference frame, facilitating intercomparison of data from a diversity of labs and instrument configurations and restandardization of a broad range of sample sets between 2006, when the first carbonate measurements were published, and the present.

Evidence of neutron leakage at the Fukushima nuclear plant from measurements of radioactive 35S in California.

A recent earthquake and the subsequent tsunami have extensively damaged the Fukushima nuclear power plant, releasing harmful radiation into the environment. Despite the obvious implication for human health and the surrounding ecology, there are no quantitative estimates of the neutron flux leakage during the weeks following the earthquake. Here, using measurements of radioactive (35)S contained in sulfate aerosols and SO(2) gas at a coastal site in La Jolla, California, we show that nearly 4 × 10(11) neutrons per m(2) leaked at the Fukushima nuclear power plant before March 20, 2011. A significantly higher (35)SO(2-)(4) activity as measured on March 28 is in accord with neutrons escaping the reactor core and being absorbed by the coolant seawater (35)Cl to produce (35)S by a (n, p) reaction. Once produced, (35)S oxidizes to (35)SO(2) and (35)SO(2-)(4) and was then transported to Southern California due to the presence of strong prevailing westerly winds at this time. Based on a moving box model, we show that the observed activity enhancement in (35)SO(2-)(4) is compatible with long-range transport of the radiation plume from Fukushima. Our model predicts that (35)SO(2-)(4), the concentration in the marine boundary layer at Fukushima, was approximately 2 × 10(5) atoms per m(3), which is approximately 365 times above expected natural concentrations. These measurements and model calculations imply that approximately 0.7% of the total radioactive sulfate present at the marine boundary layer at Fukushima reached Southern California as a result of the trans-Pacific transport.

Measurements of 129I in the Pacific Ocean at Scripps Pier and Pacific Northwest sites: A search for effects from the 2011 Fukushima Daiichi Nuclear Power Plant accident and Hanford.

Radionuclides from the Fukushima Daiichi Nuclear Power Plant were released directly into the ocean as a result of the Great East Japan Earthquake on March 11, 2011. This material became entrained in surface ocean currents and subsequently transported for great distances. In June 2011, a few months after the disaster, we began a surface ocean 129I monitoring program, with samples from Scripps Pier, La Jolla, California, USA, with the expectation that surface currents originating off the east coast of Japan would eventually carry radionuclides to the La Jolla site. After 7 years of ocean transport, a distinct signal has not yet arrived at Scripps Pier. We have however, recorded an interesting systematic seasonal 129I time series record that stems from surface circulation variations along the California coast. To provide a more comprehensive picture of the 129I budget in coastal surface waters off the west coast of the U.S., we also include 129I data from the Columbia River, and offshore sites along the coast of Washington State. Anthropogenic nuclides are carried by the Columbia River into the Pacific Ocean from the vicinity of the decommissioned Hanford nuclear facility. We find highly elevated 129I/127I values in the Columbia River, downstream from the Hanford site, but this anthropogenic 129I becomes significantly diluted once it reaches the Pacific Ocean. Nonetheless, its imprint persists in surface seawater off the west coast of the U.S. that has significantly higher 129I/127I levels than other surface sites in the Pacific Ocean.