Taioli, S; Garberoglio, G; Simonucci, S; a Beccara, S; Aversa, L; Nardi, M; Verucchi, R; ... Alfè, D; + view all Taioli, S; Garberoglio, G; Simonucci, S; a Beccara, S; Aversa, L; Nardi, M; Verucchi, R; Iannotta, S; Dapor, M; Alfè, D; - view fewer (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.

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