Mixed electric-magnetic second-order nonlinear optical response of helicenes

Edith Botek, Jean-Marie André, Benoit Champagne, Thierry Verbiest, André Persoons

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Résumé

The mixed electric-magnetic second-order nonlinear optical responses of oriented films of helicenes have been computed ab initio using the random phase approximation method and compared to the pure electric-dipole counterpart. It turns out that the mixed electric-magnetic responses can be of the same order of magnitude as the pure electric-dipole counterpart when there is no donor/acceptor (D/A) substituent or these D/A pairs are weak, i.e., when the pure electric-dipole response is small. When adding strong D/A substituents, the pure electric-dipole response increases substantially and much more than its mixed electric-magnetic counterpart. Consequently, the ratio between the mixed electric-magnetic and pure electric responses decreases. Although there is no general rule, the mixed responses evolve as a function of substitution quasi similarly to the pure electric contribution. This study confirms therefore the possibility of tuning the mixed electric-magnetic response by employing appropriate chiral molecules.

langue originaleAnglais
Numéro d'article234713
journalThe journal of chemical physics
Volume122
Numéro de publication23
Les DOIs
Etat de la publicationPublié - 15 juin 2005

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