Development, characterization, and first application of a resonant laser secondary neutral mass spectrometry setup for the research of plutonium in the context of long-term nuclear waste storage.

Plutonium is a major contributor to the radiotoxicity in a long-term nuclear waste repository; therefore, many studies have focused on interactions of plutonium with the technical, geotechnical, and geological barriers of a possible nuclear waste storage site. In order to gain new insights into the sorption on surfaces and diffusion of actinides through these complex heterogeneous materials, a highly sensitive method with spatial resolution is required. Resonant laser secondary neutral mass spectrometry (Laser-SNMS) uses the spatial resolution available in time-of-flight secondary ion mass spectrometry (TOF-SIMS) in combination with the high selectivity, sensitivity, and low background noise of resonance ionization mass spectrometry (RIMS) and is, therefore, a promising method for the study and analysis of the geochemical behavior of plutonium in long-term nuclear waste storage. The authors present an approach with a combined setup consisting of a commercial TOF-SIMS instrument and a Ti:sapphire (Ti:Sa) laser system, as well as its optimization, characterization, and improvements compared to the original proof of concept by Erdmann et al. (2009). As a first application, the spatial distributions of plutonium and other elements on the surface of a pyrite particle and a cement thin section were measured by Laser-SNMS and TOF-SIMS, respectively. These results exemplify the potential of these techniques for the surface analysis of heterogeneous materials in the context of nuclear safety research.

Penning trap mass measurements of the deuteron and the HD+ molecular ion.

The masses of the lightest atomic nuclei and the electron mass1 are interlinked, and their values affect observables in atomic2, molecular3-5 and neutrino physics6, as well as metrology. The most precise values for these fundamental parameters come from Penning trap mass spectrometry, which achieves relative mass uncertainties of the order of 10-11. However, redundancy checks using data from different experiments reveal considerable inconsistencies in the masses of the proton, the deuteron and the helion (the nucleus of helium-3), suggesting that the uncertainty of these values may have been underestimated. Here we present results from absolute mass measurements of the deuteron and the HD+ molecular ion using 12C as a mass reference. Our value for the deuteron mass, 2.013553212535(17) atomic mass units, has better precision than the CODATA value7 by a factor of 2.4 and differs from it by 4.8 standard deviations. With a relative uncertainty of eight parts per trillion, this is the most precise mass value measured directly in atomic mass units. Furthermore, our measurement of the mass of the HD+ molecular ion, 3.021378241561(61) atomic mass units, not only allows a rigorous consistency check of our results for the masses of the deuteron (this work) and the proton8, but also establishes an additional link for the masses of tritium9 and helium-3 (ref. 10) to the atomic mass unit. Combined with a recent measurement of the deuteron-to-proton mass ratio11, the uncertainty of the reference value of the proton mass7 can be reduced by a factor of three.