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Article Dans Une Revue The Journal of Chemical Physics Année : 2014

Oxygen diffusion and reactivity at low temperature on bare amorphous olivine-type silicate

Résumé

The mobility of O atoms at very low temperatures is not generally taken into account, despite O diffusion would add to a series of processes leading to the observed rich molecular diversity in space. We present a study of the mobility and reactivity of O atoms on an amorphous silicate surface. Our results are in the form of reflection absorption infrared spectroscopy and temperature-programmed desorption spectra of O$_2$ and O$_3$ produced via two pathways: O + O and O$_2$ + O, investigated in a submonolayer regime and in the range of temperature between 6.5 and 30 K. All the experiments show that ozone is formed efficiently on silicate at any surface temperature between 6.5 and 30 K. The derived upper limit for the activation barriers of O + O and O$_2$ + O reactions is ∼150 K/k$_b$. Ozone formation at low temperatures indicates that fast diffusion of O atoms is at play even at 6.5 K. Through a series of rate equations included in our model, we also address the reaction mechanisms and show that neither the Eley–Rideal nor the hot atom mechanisms alone can explain the experimental values. The rate of diffusion of O atoms, based on modeling results, is much higher than the one generally expected, and the diffusive process proceeds via the Langmuir-Hinshelwood mechanism enhanced by tunnelling. In fact, quantum effects turn out to be a key factor that cannot be neglected in our simulations. Astrophysically, efficient O$_3$ formation on interstellar dust grains would imply the presence of huge reservoirs of oxygen atoms. Since O$_3$ is a reservoir of elementary oxygen, and also of OH via its hydrogenation, it could explain the observed concomitance of CO$_2$ and H$_2$O in the ices.
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Dates et versions

hal-02555581 , version 1 (27-06-2024)

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M. Minissale, E. Congiu, F. Dulieu. Oxygen diffusion and reactivity at low temperature on bare amorphous olivine-type silicate. The Journal of Chemical Physics, 2014, 140 (7), pp.074705. ⟨10.1063/1.4864657⟩. ⟨hal-02555581⟩
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