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Ces dernières années, les agrégats d’hélium superfluides ont fait l’objet de nombreuses études aussi bien expérimentales que théoriques. Le fruit de ces études a permis le développement de méthodes spectroscopiques innovantes (HENDI) utilisant les nanogouttes d’hélium comme l’ultime matrice, exploitant ainsi la très faible température de ce milieu particulier et sa faible interaction avec les dopants pour une meilleure résolution spectrale. Cependant, un nombre important de questions subsiste quant aux agrégats d’hélium dopés, particulièrement, ceux dopés par les alcalino-terreux. En effet, la position d’une impureté au sein de la gouttelette d’hélium est loin d’être un problème trivial pour certaines espèces telles les alcalino-terreux. Ceci est particulièrement vrai dans le cas où l’impureté est l’atome de magnésium. Des preuves expérimentales d’un état solvaté du magnésium sont annoncées dans la littérature tandis que de récentes expériences laissent penser à une position plutôt surfacique du magnésium dans les agrégats d’hélium. Du point de vue théorique, la même ambiguïté persiste quant à la position de Mg dans la nanogoutte d’hélium. Dans le but de contribuer à une meilleure compréhension des clusters d’hélium dopés par les métaux alcalino-terreux (Mg et Ca), nous avons, au cours de ce travail, dû déterminer avec précision les énergies d’interactions des états fondamentaux des systèmes van der Waals CaHe et MgHe. Pour ce faire, des méthodes ab initio telles les approches des clusters couplés (CC) mais aussi perturbationnelles (MP2 et MP4) ont été appliquées à ces deux systèmes avec succès. Les meilleurs potentiels d’interaction ont été utilisés par la suite comme potentiels d’interactions de paire dans l’approche Monte Carlo à diffusion (DMC) en combinaison de deux types de potentiel d’interaction pour l’hélium. Aussi bien pour CaHen que pour MgHen, des simulations DMC ont été produites depuis n = 1 jusqu’à n = 220, le résultat principal en est une position surfacique de l’impureté quelque soit l’alcalino-terreux considéré. Dans le cas particulièrement délicat des clusters d’hélium dopés par le magnésium, des calculs de DMC avec des contraintes géométriques montrent que le potentiel radial effectif de Mg dans He20 et He50 est plutôt plat. Enfin, sont présentés également les résultats concernant la recombinaison dynamique de deux atomes de magnésium à l’intérieur d’un agrégat d’environ 2000 atomes d’hélium utilisant une méthode basée sur un potentiel effectif pour l’interaction He-He / During the last decades, superfluid helium clusters have been widely studied both experimentally and theoretically. As a result of the latter studies, a new spectroscopic domain has emerged (HENDI) where helium nanodroplets are used as ultimate matrices for accurate spectroscopic measurements, taking advantage of their very low temperature and their weak interaction with the impurity. However, many questions still are remaining about the helium nanodroplets, especially those doped with alkaline-earth atoms. In fact, the simple position of an impurity in this medium is far from being trivial for some doping species like the alkaline-earth atoms. This is particularly true when the impurity is the magnesium atom. Experimental evidence of a completely Mg solvated state is announced in the literature whereas very recent experiments advance the opposite situation for the Mg atom (near the surface). From the theoretical point of view, the position of the Mg atom in the helium droplet still remain ambiguous in the actual literature. In order to contribute to a better understanding of the alkaline-earth (Mg and Ca) doped helium clusters, we have determined, in this work, accurate interaction energies for both CaHe and MgHe van der Waals systems. For this aim, ab initio methods such as the coupled clusters (CC) as well as Møller-Plesset approaches (MP2 and MP4) have been successfully applied to both systems. The best interaction potentials have been then used as pair interactions for the diffusion Monte Carlo (DMC) approach in combination with two accurate helium pair interactions. For both CaHen and MgHen, DMC calculations have been carried out for n = 1 up to 220, the result was a surface location of the dopant whatever the latter is. In the particularly delicate case of Mg doped helium clusters, constrained DMC calculations have been performed for He20 and He50. The results were a very flat energy profile in both cases. Finally, results concerning the dynamics of recombination of two Mg atoms based on an effective potential for helium inside an almost 2000 helium atom cluster are given

The decay of quantum turbulence in superfluid (_^4)He in the zero temperature limit wasinvestigated. Quantum turbulence was created by impulsive spin-down from a specific angular velocity to rest. A measurement of the vortex line density was performed using the scattering of charged vortex rings. The vortex line density decayed as L ∝ t^(-3/2) which is the characteristic of quasiclassical turbulence forced at large length scales. The interaction of metastable spin-triplet 〖He〗_2^* molecules with quantized vortex lines in superfluid (_^4)He at temperatures below 200 mK was studied too. The molecules were generated during an injection of electrons from a sharp metal tip at high voltage. They were detected as a current into a metal collector after ionization upon colliding with the collector surface. The detected current was suppressed by even a small rotation indicating the trapping of the molecules on quantized vortices. The presence of (_^3)He impurities at the level of 0.3 ppb strongly suppressed the detected signal. The temperature dependence of the detected signal showed a sharp peak, most probably associated with the condensation of (_^3)He atoms on vortex cores. The time of flight of the molecules as a function of temperature was measured. It was observed that there are three regimes for 〖He〗_2^* molecules transportation in superfluid (_^4)He : ballistic regime for T < 100 mK, diffusive for T > 200 mK, and an intermediate regime between them. The vortex lines were created by either rotation or ion injection. The trapping diameter of the molecules on quantized vortices was found to be 96 ± 6 nm at pressure of 0.1 bar and 27 ± 5 nm at 5.0 bar. It was also demonstrated that a tangle of vortices moving in superfluid (_^4)He are capable of conveying the 〖He〗_2^* molecules through the drift region.

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This project’s goal is to evaluate the use of groundwater Rn as a tool for the search of deeply buried U deposits. To do so, the concentrations of major cations, anions, Rn, 4He, and 3H were measured in groundwater. Additionally, the abundance, composition, and distribution of radionuclides (U, Ra, 206Pb, 207Pb, 208Pb), were measured in soil and sandstone above the Denison Mines’ Phoenix Deposit (located at a depth of ~450 m). Rn was extracted from groundwater using mineral oil, and higher groundwater Rn radioactivity (average 0.13 Bq/g of water, n=10) was found in drill holes within ~100 meters of the Phoenix Deposit’s surface projection than in distal holes (average 0.072 Bq/g of oil, n=4). High Rn radioactivity is independent of the drill holes’ intersection with U ore, indicating that drilling did not transport significant amounts of Rn or parent isotopes to shallow depths. The water table is commonly within the Dunlop Member of the Athabasca sandstones, and groundwater Rn is positively correlated with average U concentrations obtained by modified aqua regia digestion of sandstones (analytical code 2AMS at the Saskatchewan Research Council) and also positively correlated with U in three-acid digestion of sandstones (analytical code 3AMS at the Saskatchewan Research Council). Diffusion models show Rn cannot travel significant distances, and so Rn is likely produced in MFd from the in-situ decay of U and Ra. 226Ra radioactivity was measured for B horizon soil samples (n=39) and sandstone samples (n=20) after a HCl leach followed with BaSO4 precipitation. An extraction efficiency for Ra of 28.2%±3.8%. was determined by comparing the soil BaSO4 precipitation procedure against unprocessed soils. Ra radioactivity in B horizon soil is lower than expected from U contents determined with INAA. Ra radioactivity is comparable to the values expected from INAA U concentrations (n=17) in sandstone, with exception to 4 Dunlop Member samples and 2 samples in the Read Formation and Bird Member. Ra in 4 of 5 samples in the Dunlop Member are 10-50% overabundant, perhaps resulting from Ra percolating downwards from soil. The proposed interpretation is consistent with lower than expected Ra radioactivity of B horizon soil. Ra is 260% and 420% overabundant in the two samples from the Read Formation and the Bird Member (1 each), suggesting upward migration of Ra from the U deposit. Low solute concentration and a neutral-weakly alkaline pH of shallow groundwater in the study area appears to prevent significant travel of Ra ions through groundwater by means of ion absorption competition. Pb isotopic compositions were determined using an ICP-MS for sandstones and soil via three different leaches; 0.02 N HBr, 2.7 N HCl, and concentrated HBr. Overall, Pb isotopic compositions of MFd (n=5) and B horizon (n=10) are similar, supporting the percolation of acidic surface waters through soil. One sample from RD (among 4 samples) show high 206Pb, suggesting an upward migration of 206Pb from the deposit. The ratios of 4He/3He in ground water ranged between 0.95-1.07; typical of groundwater-atmosphere interaction. The lateral flow of groundwater at deep levels can explain the absence of higher 4He/3He.

Spectroscopic measurements of the helium atom are performed to high precision using an atomic beam apparatus and electro-optic laser techniques. These measurements, in addition to serving as a test of helium theory, also provide a new determination of the fine structure constant &#945;. An apparatus was designed and built to overcome limitations encountered in a previous experiment. Not only did this allow an improved level of precision but also enabled new consistency checks, including an extremely useful measurement in 3He. I discuss the details of the experimental setup along with the major changes and improvements. A new value for the J = 0 to 2 fine structure interval in the 23P state of 4He is measured to be 31 908 131.25(30) kHz. The 300 Hz precision of this result represents an improvement over previous results by more than a factor of three. Combined with the latest theoretical calculations, this yields a new determination of &#945; with better than 5 ppb uncertainty, &#945;-1 = 137.035 999 55(64).

The thermodynamics inside the helium liquefier in the FREIA laboratory still contains many unknowns. The purpose of this project is to develop a theoretical model and implement it in MATLAB, with the help of the CoolProp library. This theoretical model of the FREIA liquefaction cycle aims at finding the unknown parameters not specified in the manual of the manufacturer, starting from the principle of enthalpy conservation. Inspiration was taken from the classical liquefaction cycles of Linde-Hampson, Claude and Collins. We developed a linear mathematical model for cycle components such as turboexpanders and heat exchangers, and a non-linear model for the liquefaction in the phase separator. Liquefaction yields of 10% and 6% were obtained in our model simulations, with and without liquid nitrogen pre-cooling respectively - similar to those in the FREIA liqueuefier within one percentage point. The sensors placed in FREIA showed similar pressure and temperature values, even though not every point could be verified due to the lack of sensors. We observed an increase of more than 50% in yield after adjustments of the heat exchanger design in the model, especially the first one. This constitutes a guideline for possible future improvements of the liquefier. / Termodynamiken bakom heliumförvätskaren i FREIA-laboratoriet innehåller fortfarande många okända aspekter. Detta kandidatarbete syftar till att utveckla en teoretisk modell och implementera den i MATLAB med hjälp av biblioteket CoolProp. Denna modell av FREIA:s förvätskningscykel syftar till att hitta de okända parametrar som inte specificerats av tillverkaren, och baserar sig på principen om entalpins bevarande. Inspiration togs från de klassiska förvätskningscyklerna Linde-Hampson, Claude och Collins. Vi utvecklade en linjär matematisk modell för cykelkomponenter såsom expansionsturbiner och värmeväxlare, och en icke-linjär modell för själva förvätskningen i fasseparatorn. En förvätskningsverkningsgrad på 10% och 6% uppnåddes i våra modellsimuleringar, med respektive utan förkylning med flytande kväve - liknande verkningsgraderna i FREIA- förvätskaren inom en procentenhet. Sensorerna placerade i FREIA visade på liknande tryck och temperaturer, även om bristen på sensorer gjorde att vi inte kunde bekräfta varje punkt. Vi observerade en ökning på mer än 50% i verkningsgrad efter att ha justerat värmeväxlardesignen något, speciellt för den första. Detta kan utgöra riktlinjer för var man framöver kan förbättra den faktiska förvätskaren. / <p>Subject reader/Ämnesgranskare: Roger Ruber</p>

abstract: A mineral’s helium content reflects a balance between two competing processes: accumulation by radioactive decay and temperature-dependent diffusive loss. (U-Th)/He dating of zircon and other uranium and thorium-bearing minerals provides insight into the temperature histories of rocks at or near Earth’s surface that informs geoscientists’ understanding of tectonic and climate-driven exhumation, magmatic activity, and other thermal events. The crystal structure and chemistry of minerals affect helium diffusion kinetics, recorded closure temperatures, and interpretations of (U-Th)/He datasets. I used empirical and experimental methods to investigate helium systematics in two minerals chronometers: zircon and xenotime. The same radioactivity that makes zircon a valuable chronometer damages its crystal structure over time and changes zircon helium kinetics. I used a zircon, titanite, and apatite (U-Th)/He dataset combined with previously published data and a new thermal model to place empirical constraints on the closure temperature for helium in a suite of variably damaged zircon crystals from the McClure Mountain syenite of Colorado. Results of this study suggest that the widely-used zircon damage accumulation and annealing model (ZRDAAM) does not accurately predict helium closure temperatures for a majority of the dated zircons. Detailed Raman maps of Proterozoic zircon crystals from the Lyon Mountain Granite of New York document complex radiation damage zoning. Models based on these results suggest that most ancient zircons are likely to exhibit intracrystalline variations in helium diffusivity due to radiation damage zoning, which may, in part, explain discrepancies between my empirical findings and ZRDAAM. Zircon crystallography suggests that helium diffusion should be fastest along the crystallographic c-axis. I used laser depth profiling to show that diffusion is more strongly anisotropic than previously recognized. These findings imply that crystal morphology affects the closure temperature for helium in crystalline zircon. Diffusivity and the magnitude of diffusive anisotropy decrease with low doses of radiation damage. Xenotime would make a promising (U-Th)/He thermochronometer if its helium kinetics were better known. I performed classic step-wise degassing experiments to characterize helium diffusion in xenotime FPX-1. Results suggest that this xenotime sample is sensitive to exceptionally low temperatures (∼50 °C) and produces consistent (U-Th)/He dates. / Dissertation/Thesis / Doctoral Dissertation Geological Sciences 2019