A density functional tight binding/force field approach to the interaction of molecules with rare gas clusters: Application to (C6H6)+/0Ar n clusters - Archive ouverte HAL Accéder directement au contenu
Article Dans Une Revue Journal of Chemical Physics Année : 2014

A density functional tight binding/force field approach to the interaction of molecules with rare gas clusters: Application to (C6H6)+/0Ar n clusters

Résumé

We propose in the present paper a SCC-DFTB/FF (Self-Consistent-Charge Density Functional based Tight Binding/Force-Field) scheme adapted to the investigation of molecules trapped in rare gas environments. With respect to usual FF descriptions, the model involves the interaction of quantum electrons in a molecule with rare gas atoms in an anisotropic scheme. It includes polarization and dispersion contributions and can be used for both neutral and charged species. Parameters for this model are determined for hydrocarbon-argon complexes and the model is validated for small hydrocarbons. With the future aim of studying polycyclic aromatic hydrocarbons in Ar matrices, extensive benchmark calculations are performed on (C6H6)+/0Ar n clusters against DFT and CCSD(T) calculations for the smaller sizes, and more generally against other experimental and theoretical data. Results on the structures and energetics (isomer ordering and energy separation, cohesion energy per Ar atom) are presented in detail for n = 1-8, 13, 20, 27, and 30, for both neutrals and cations. We confirm that the clustering of Ar atoms leads to a monotonous decrease of the ionization potential of benzene for n ⩽ 20, in line with previous experimental and FF data.
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Dates et versions

hal-00935781 , version 1 (24-01-2014)

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Christophe Iftner, Aude Simon, Kseniia Korchagina, Mathias Rapacioli, Fernand Spiegelman. A density functional tight binding/force field approach to the interaction of molecules with rare gas clusters: Application to (C6H6)+/0Ar n clusters. Journal of Chemical Physics, 2014, 140, pp.034301. ⟨10.1063/1.4861431⟩. ⟨hal-00935781⟩
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