Demonstration of tritium adsorption on graphene.

In this work, we report on studies of graphene exposed to tritium gas in a controlled environment. The single layer graphene on a SiO2/Si substrate was exposed to 400 mbar of T2, for a total time of ∼55 h. The resistivity of the graphene sample was measured in situ during tritium exposure using the van der Pauw method. We found that the sheet resistance increases by three orders of magnitude during the exposure, suggesting significant chemisorption of tritium. After exposure, the samples were characterised ex situ via spatio-chemical mapping with a confocal Raman microscope, to study the effect of tritium on the graphene structure (tritiation yielding T-graphene), as well as the homogeneity of modifications across the whole area of the graphene film. The Raman spectra after tritium exposure were comparable to previously observed results in hydrogen-loading experiments, carried out by other groups. By thermal annealing we also could demonstrate, using Raman spectral analysis, that the structural changes were largely reversible. Considering all observations, we conclude that the graphene film was at least partially tritiated during the tritium exposure, and that the graphene film by and large withstands the bombardment by electrons from the ß-decay of tritium, as well as by energetic primary and secondary ions.

Versatile Confocal Raman Imaging Microscope Built from Off-the-Shelf Opto-Mechanical Components.

Confocal Raman microscopic (CRM) imaging has evolved to become a key tool for spatially resolved, compositional analysis and imaging, down to the µm-scale, and nowadays one may choose between numerous commercial instruments. That notwithstanding, situations may arise which exclude the use of a commercial instrument, e.g., if the analysis involves toxic or radioactive samples/environments; one may not wish to render an expensive instrument unusable for other uses, due to contamination. Therefore, custom-designed CRM instrumentation-being adaptable to hazardous conditions and providing operational flexibility-may be beneficial. Here, we describe a CRM setup, which is constructed nearly in its entirety from off-the-shelf optomechanical and optical components. The original aim was to develop a CRM suitable for the investigation of samples exposed to tritium. For increased flexibility, the CRM system incorporates optical fiber coupling to both the Raman excitation laser and the spectrometer. Lateral raster scans and axial profiling of samples are facilitated by the use of a motorized xyz-translation assembly. Besides the description of the construction and alignment of the CRM system, we also provide (i) the experimental evaluation of system performance (such as, e.g., spatial resolution) and (ii) examples of Raman raster maps and axial profiles of selected thin-film samples (such as, e.g., graphene sheets).

Accurate Reference Gas Mixtures Containing Tritiated Molecules: Their Production and Raman-Based Analysis.

Highly accurate, quantitative analyses of mixtures of hydrogen isotopologues-both the stable species, H2, D2, and HD, and the radioactive species, T2, HT, and DT-are of great importance in fields as diverse as deuterium-tritium fusion, neutrino mass measurements using tritium ß-decay, or for photonuclear experiments in which hydrogen-deuterium targets are used. In this publication we describe a production, handling, and analysis facility capable of fabricating well-defined gas samples, which may contain any of the stable and radioactive hydrogen isotopologues, with sub-percent accuracy for the relative species concentrations. The production is based on precise manometric gas mixing of H2, D2, and T2. The heteronuclear isotopologues HD, HT, and DT are generated via controlled, in-line catalytic reaction or by ß-induced self-equilibration, respectively. The analysis was carried out using an in-line intensity- and wavelength-calibrated Raman spectroscopy system. This allows for continuous monitoring of the composition of the circulating gas during the self-equilibration or catalytic evolution phases. During all procedures, effects, such as exchange reactions with wall materials, were considered with care. Together with measurement statistics, these and other systematic effects were included in the determination of composition uncertainties of the generated reference gas samples. Measurement and calibration accuracy at the level of 1% was achieved.