Taioli, S;
Garberoglio, G;
Simonucci, S;
a Beccara, S;
Aversa, L;
Nardi, M;
Verucchi, R;
... Alfè, D; + view all
(2013)
Non-adiabatic ab initio molecular dynamics of supersonic beam epitaxy of silicon carbide at room temperature.
J Chem Phys
, 138
(4)
, Article 044701. 10.1063/1.4774376.
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Abstract
In this work, we investigate the processes leading to the room-temperature growth of silicon carbide thin films by supersonic molecular beam epitaxy technique. We present experimental data showing that the collision of fullerene on a silicon surface induces strong chemical-physical perturbations and, for sufficient velocity, disruption of molecular bonds, and cage breaking with formation of nanostructures with different stoichiometric character. We show that in these out-of-equilibrium conditions, it is necessary to go beyond the standard implementations of density functional theory, as ab initio methods based on the Born-Oppenheimer approximation fail to capture the excited-state dynamics. In particular, we analyse the Si-C(60) collision within the non-adiabatic nuclear dynamics framework, where stochastic hops occur between adiabatic surfaces calculated with time-dependent density functional theory. This theoretical description of the C(60) impact on the Si surface is in good agreement with our experimental findings.
| Type: | Article |
|---|---|
| Title: | Non-adiabatic ab initio molecular dynamics of supersonic beam epitaxy of silicon carbide at room temperature |
| Location: | United States |
| Open access status: | An open access version is available from UCL Discovery |
| DOI: | 10.1063/1.4774376 |
| Publisher version: | http://dx.doi.org/10.1063/1.4774376 |
| Language: | English |
| Additional information: | © 2013 Author(s). Published through AIP's Author Select initiative under the terms of the Creative Commons 3.0 Unported License. |
| Keywords: | Carbon Compounds, Inorganic, Molecular Dynamics Simulation, Quantum Theory, Silicon Compounds, Temperature |
| UCL classification: | UCL UCL > Provost and Vice Provost Offices > UCL BEAMS UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences > Dept of Earth Sciences |
| URI: | https://discovery.ucl.ac.uk/id/eprint/1386546 |
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