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1.
Phys Rev Lett ; 111(5): 053201, 2013 Aug 02.
Article in English | MEDLINE | ID: mdl-23952395

ABSTRACT

Any evolving system can change state via thermal mechanisms (hopping a barrier) or via quantum tunneling. Most of the time, efficient classical mechanisms dominate at high temperatures. This is why an increase of the temperature can initiate the chemistry. We present here an experimental investigation of O-atom diffusion and reactivity on water ice. We explore the 6-25 K temperature range at submonolayer surface coverages. We derive the diffusion temperature law and observe the transition from quantum to classical diffusion. Despite the high mass of O, quantum tunneling is efficient even at 6 K. As a consequence, the solid-state astrochemistry of cold regions should be reconsidered and should include the possibility of forming larger organic molecules than previously expected.

2.
J Chem Phys ; 137(23): 234706, 2012 Dec 21.
Article in English | MEDLINE | ID: mdl-23267497

ABSTRACT

The formation of the first monolayer of water molecules on bare dust grains is of primary importance to understand the growth of the icy mantles that cover dust in the interstellar medium. In this work, we explore experimentally the formation of water molecules from O(2) + D reaction on bare silicate surfaces that simulates the grains present in the diffuse interstellar clouds at visual extinctions (A(V) < 3 mag). For comparison, we also study the formation of water molecules on surfaces covered with amorphous water ice representing the dense clouds (A(V) ≥ 3 mag). Our studies focus on the formation of water molecules in the sub-monolayer and monolayer regimes using reflection absorption infrared spectroscopy and temperature-programmed desorption techniques. We provide the fractions of the products, such as D(2)O and D(2)O(2) molecules formed on three astrophysically relevant surfaces held at 10 K (amorphous olivine-type silicate, porous amorphous water ice, and nonporous amorphous water ice). Our results showed that the formation of D(2)O molecules occurs with an efficiency of about 55%-60% on nonporous amorphous water ice and about 18% on bare silicate grains surfaces. We explain the low efficiency of D(2)O water formation on the silicate surfaces by the desorption upon formation of certain products once the reaction occurs between O(2) and D atoms on the surface. A kinetic model taking into account the chemical desorption of newly formed water supports our conclusions.

3.
J Phys Chem A ; 111(49): 12611-9, 2007 Dec 13.
Article in English | MEDLINE | ID: mdl-17988107

ABSTRACT

The study of the formation of molecular hydrogen on low-temperature surfaces is of interest both because it enables the exploration of elementary steps in the heterogeneous catalysis of a simple molecule and because of its applications in astrochemistry. Here, we report results of experiments of molecular hydrogen formation on amorphous silicate surfaces using temperature-programmed desorption (TPD). In these experiments, beams of H and D atoms are irradiated on the surface of an amorphous silicate sample. The desorption rate of HD molecules is monitored using a mass spectrometer during a subsequent TPD run. The results are analyzed using rate equations, and the energy barriers of the processes leading to molecular hydrogen formation are obtained from the TPD data. We show that a model based on a single isotope provides the correct results for the activation energies for diffusion and desorption of H atoms. These results are used in order to evaluate the formation rate of H2 on dust grains under the actual conditions present in interstellar clouds. It is found that, under typical conditions in diffuse interstellar clouds, amorphous silicate grains are efficient catalysts of H2 formation when the grain temperatures are between 9 and 14 K. This temperature window is within the typical range of grain temperatures in diffuse clouds. It is thus concluded that amorphous silicates are good candidates to be efficient catalysts of H2 formation in diffuse clouds.

4.
Nature ; 438(7069): 785-91, 2005 Dec 08.
Article in English | MEDLINE | ID: mdl-16319827

ABSTRACT

On the basis of previous ground-based and fly-by information, we knew that Titan's atmosphere was mainly nitrogen, with some methane, but its temperature and pressure profiles were poorly constrained because of uncertainties in the detailed composition. The extent of atmospheric electricity ('lightning') was also hitherto unknown. Here we report the temperature and density profiles, as determined by the Huygens Atmospheric Structure Instrument (HASI), from an altitude of 1,400 km down to the surface. In the upper part of the atmosphere, the temperature and density were both higher than expected. There is a lower ionospheric layer between 140 km and 40 km, with electrical conductivity peaking near 60 km. We may also have seen the signature of lightning. At the surface, the temperature was 93.65 +/- 0.25 K, and the pressure was 1,467 +/- 1 hPa.

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