Laser Spectroscopic Measurement of Helium Isotope Ratios

A sensitive laser spectroscopic method has been applied to the quantitative determination of the isotope ratio of helium at the level of 3He/4He = 10^-7 - 10^-5. The resonant absorption of 1083 nm laser light by the metastable 3He atoms in a discharge cell was measured with the frequency modulation saturation spectroscopy technique while the abundance of 4He was measured by a direct absorption technique. The results on three different samples extracted from the atmosphere and commercial helium gas were in good agreement with values obtained with mass spectrometry. The achieved 3-sigma detection limit of 3He in helium is 4 x 10^-9. This demonstration required a 200 micro-L STP sample of He. The sensitivity can be further improved, and the required sample size reduced, by several orders of magnitude with the addition of cavity enhanced spectroscopy

Accurate determination of the absolute 3He/4He ratio of a synthesized helium standard gas (Helium Standard of Japan, HESJ): Towards revision of the atmospheric 3He/4He ratio

The helium standard of Japan, referred to as HESJ, is an inter-laboratory standard for the 3He/4He ratio. While the ratio of 3He and 4He of the HESJ was previously determined by a relative comparison to atmospheric helium, the absolute value of the 3He/4He ratio of the HESJ has not been directly determined yet. Therefore, it relies on the early measurements of that of atmospheric helium. The accuracy of the absolute 3He/4He ratios of the atmosphere and other working standards including HESJ is crucial in some applications of helium isotopes, such as tritium-3He dating, surface-exposure age determination based on cosmogenic 3He, and the accurate measurement of the neutron lifetime. In this work, new control samples of helium gases with 3He/4He ratios of 14, 28, and 42 ppm were fabricated with accuracy of 0.25-0.38% using a gas-handling system for a neutron lifetime experiment at Japan Proton Accelerator Research Complex (J-PARC). The relative 3He/4He ratios of these samples and the HESJ were measured using a magnetic-sector-type, single-focusing, noble gas mass spectrometer with a double collector system. As a result, the absolute 3He/4He ratio of the HESJ was determined as 27.36 +/- 0.11 ppm. The atmospheric 3He/4He ratio was determined as 1.340 +/- 0.006 ppm, based on this work.Comment: 18 pages, 8 figures, 4 table

Isotope composition of helium in ultrabasic xenoliths from volcanic rocks of Kamchatka

The purpose of this work is to refine our knowledge about the nature of helium with a high abundance of the rare isotope3He(3He/4He= 10−5) discovered in terrestrial volcanic gases in 1968. We will discuss here the results of isotope analyses of helium released by step-wise heating of ultrabasic xenoliths and some volcanic rocks. On the basis of these results, possible sources of3He in the earth due to fission and nuclear reactions are considered critically. The most probable source of the high abundance of3He is shown to be due to the capture and trapping of primordial He by the earth during its formation (primordial helium3He/4He= 3 × 10−4), a small but significant fraction of which has been retained to the present time

Amphibole: A major carrier of helium isotopes in crustal rocks

The first evidence for a specific role of amphiboles in He isotope balance of crustal rocks was presented in early contributions by Gerling et al. (1971, 1976). Since then it was shown that 4He and 3He concentrations in amphiboles generally exceed those in the host rock samples. Recently amphibole was considered as an important carrier of noble gases and other volatiles components in the course of their subduction into the mantle. This paper presents new data on the balance and mobility of noble gas isotopes and major gas constituents in amphibole separates in order to understand sources and evolution of volatile components of 2666 Ma old alkaline granites from Ponoy massif (Kola Peninsula), which underwent metamorphism 1802 Ma ago.In the amphiboles 3He, 4He and 40Ar* were dominantly produced in situ due to radioactive decay of the parent isotopes and associated nuclear reactions. A small fraction of He (≈ 3% of the total) is liberated by crushing and shows 3He/4He ratio indistinguishable from that found by total extraction. The fraction of trapped 40Ar* amounts to ≈ 40%; both these fractions presumably occupy fluid inclusions and show rather low 4He/40Ar* ≈ 0.1, a factor of ≈ 150 below the production ratio (calculated assuming no loss / gain of the species has happened since the time of metamorphism).3He has been better preserved in amphiboles compared with 4He: the retention parameter (measured amount of He / totally produced amount) for 3He (≈ 0.4) exceeds that for 4He (≈ 0.15).He extraction by fast and slow linear heating of amphiboles resulted in different release patterns. The fast heating (within 12 to 40 °C min− 1) revealed a superposition of two peaks. When heating with slower heating rate (below 8 °C min− 1) was applied, the high-temperature peak disappeared (the “disappearing site”). Extractions of He atoms from grain and powder samples at different heating rates have shown that: (1) the “disappearing site” is revealed by the fast heating analyses of different amphibole samples but not only those from the Ponoy massif; (2) amount of He liberated from the “disappearing site” is variable and generally much less than the total amount of He in the sample; (3) analysis of the powder produced in the crushing experiments never reveals the “disappearing site”; the temperature of He release from the powder is lower than that from the mm grain size sample by ≈ 50 °C. Possible explanations of the nature of the “disappearing site” are discussed. However, independently on nature of this effect, repeated gas extractions by heating at different rates would give additional information about structure and its transformation during heating of amphiboles.The simplest explanation of the observed abundances of noble gas isotopes in the amphibole separates from Ponoy granites suggests local production, redistribution and partial loss of noble gases during evolution of the massif

Critical Review of Theoretical Models for Anomalous Effects (Cold Fusion) in Deuterated Metals

We briefly summarize the reported anomalous effects in deuterated metals at ambient temperature, commonly known as "Cold Fusion" (CF), with an emphasis on important experiments as well as the theoretical basis for the opposition to interpreting them as cold fusion. Then we critically examine more than 25 theoretical models for CF, including unusual nuclear and exotic chemical hypotheses. We conclude that they do not explain the data.Comment: 51 pages, 4 Figure

The Inherent Tracer Fingerprint of Captured CO2.

Carbon capture and storage (CCS) is the only currently available technology that can directly reduce anthropogenic CO2 emissions arising from fossil fuel combustion. Monitoring and verification of CO2 stored in geological reservoirs will be a regulatory requirement and so the development of reliable monitoring techniques is essential. The isotopic and trace gas composition - the inherent fingerprint - of captured CO2 streams is a potentially powerful, low cost geochemical technique for tracking the fate of injected gas in CCS projects; carbon and oxygen isotopes, in particular, have been used as geochemical tracers in a number of pilot CO2 storage sites, and noble gases are known to be powerful tracers of natural CO2 migration. However, the inherent tracer fingerprint in captured CO2 streams has yet to be robustly investigated and documented and key questions remain, including how consistent is the fingerprint, what controls it, and will it be retained en route to and within the storage reservoir? Here we present the first systematic measurements of the carbon and oxygen isotopes and the trace noble gas composition of anthropogenic CO2 captured from combustion power stations and fertiliser plants. The analysed CO2 is derived from coal, biomass and natural gas feedstocks, using amine capture, oxyfuel and gasification processes, from six different CO2 capture plants spanning four different countries. We find that δ13C values are primarily controlled by the δ13C of the feedstock while δ18O values are predominantly similar to atmospheric O2. Noble gases are of low concentration and exhibit relative element abundances different to expected reservoir baselines and air, with isotopic compositions that are similar to air or fractionated air. The use of inherent tracers for monitoring and verification was provisionally assessed by analysing CO2 samples produced from two field storage sites after CO2 injection. These experiments at Otway, Australia, and Aquistore, Canada, highlight the need for reliable baseline data. Noble gas data indicates noble gas stripping of the formation water and entrainment of Kr and Xe from an earlier injection experiment at Otway, and inheritance of a distinctive crustal radiogenic noble gas fingerprint at Aquistore. This fingerprint can be used to identify unplanned migration of the CO2 to the shallow subsurface or surface

Impact ionization mass spectra of anorthite cosmic dust analogue particles

Anorthite, the Ca-rich end-member of plagioclase feldspar, is a dominant mineral component of the Lunar highlands. Plagioclase feldspar is also found in comets, meteorites and stony asteroids. It is therefore expected to contribute to the population of interplanetary (and circumplanetary) dust grains within the solar system. After coating micron- and submicron-sized grains of Anorthite with a conductive layer of Platinum, the mineral was successfully accelerated to hypervelocity speeds in the Max Planck Institut für Kernphysik’s Van de Graaff accelerator. We present impact ionization mass spectra generated following the impacts of anorthite grains with a prototype mass spectrometer (the Large Area Mass Analyser, LAMA) designed for use in space, and discuss the behavior of the spectra with increasing impact energy. Correlation analysis is used to identify the compositions and sources of cations present in the spectra, enabling the identification of several molecular cations (e.g., CaAlO2, CaSiO2, Ca2AlO3/CaAlSi2O2) which identify anorthite as the progenitor bulk grain material