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Echanges hydrogène/deutérium dans les glaces interstellaires : une origine de la deutération sélective

Abstract : The interstellar medium where stars are formed consists of a dilute gas which is dominated by molecular hydrogen and dust grains less than a few microm in size. The dust plays a crucial role in the attenuation of light from the stars. They also protect molecules within the gas from UV photons. Furthermore, they serve as heterogeneous catalysts for chemistry at low temperature. The surface of the grains also permit the formation of complex organic molecules such as methanol via the hydrogenation and/or deuteration of carbon monoxide. The ices are formed and subsequently participate in increasing the molecular complexity of the clouds. Finally, they are incorporated into debris disks, asteroids, comets, and exoplanets. The objective of this thesis is to study the mechanism of hydrogen/deuterium exchange within certain functionnal groups of simple organic molecules such as methanol, which are present on the surface of these grain mantles. The thesis is focused on the experimental determination of these processes in the condensed phase. This will be achieved with the aid of a cryogenic synthesis of the ices at very low temperatures coupled with infrared spectrometry. We observe that it is possible for the exchange to proceed before the sublimation of the ice mantles. However, this is only the case when the functional groups within the molecule may form hydrogen bonds with water. From our results we see that this process seems to be catalysed by the crystalization of the water ice. The kinetics study permits us to evalute the activation energy for the H/D exchange (6745 K) and for the transition from amorphous to crystaline ice (8100 K). In addition it also allows us to determine the rate constant for the exchange in the temperature range 120-140 K. In addition we have performed theoretical calulation in an attempt to elucidate the mechanism for the exchange. However, the experimental rate constant for the exchange is much larger in comparison to the one predicted by a semi- classical treatment based on the AB initio potential we have obtained. Further to this observations of methanol towards protostars have been conducted. These observations show that there is a variation in the relative abundance of the CH2DOH and CH3OD. This variation in relative abundance seems to have some dependence upon the mass of the protostar, with high mass stars showing (CH2DOH/CH3OD ≤ 1) and low/intermiediate mass stars showing (CH2DOH/CH3OD >> 3).
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Submitted on : Wednesday, December 19, 2012 - 3:57:54 PM
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Alexandre Ratajczak. Echanges hydrogène/deutérium dans les glaces interstellaires : une origine de la deutération sélective. Autre [cond-mat.other]. Université de Grenoble, 2012. Français. ⟨NNT : 2012GRENY014⟩. ⟨tel-00767169⟩



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