Origin of the surface-induced first hyperpolarizability in the C 60/SiO2 system: SCC-DFTB insight

Sébastien Nénon, Benoit Champagne

Résultats de recherche: Contribution à un journal/une revueArticleRevue par des pairs


Using the self-consistent charge density functional tight binding (SCC-DFTB) method, C60 molecules physisorbed on an α-quartz slab are shown to display a first hyperpolarizability, whereas, owing to their symmetry, both the α-quartz slab and C60 molecule have no first hyperpolarizabilities. A larger first hyperpolarizability is achieved when the lowest-lying (five- or six-membered) ring is situated in between two hydroxyl rows, rather than on top, because this situation favors orbital overlaps and charge transfer. Further analysis has demonstrated that (i) the first hyperpolarizability originates from the MO overlap and field-induced charge transfers from the neighboring substrate/adsorbate moieties but not to geometric relaxation of the C60 molecules at the interface and that (ii) larger first hyperpolarizabilities are associated with low surface coverage and with small distances between C60 and the surface. This contribution is a clear illustration of the emergence of second-order nonlinear optical responses (first hyperpolarizability) as a result of breaking the centrosymmetry.

langue originaleAnglais
Pages (de - à)149-153
Nombre de pages5
journalJournal of Physical Chemistry Letters
Numéro de publication1
Les DOIs
Etat de la publicationPublié - 2 janv. 2014

Empreinte digitale

Examiner les sujets de recherche de « Origin of the surface-induced first hyperpolarizability in the C 60/SiO2 system: SCC-DFTB insight ». Ensemble, ils forment une empreinte digitale unique.

Contient cette citation