Surface enhanced second harmonic generation from macrocycle, catenane, and rotaxane thin films: experiments and theory

Imad ARFAOUI, Veronica BERMUDEZ, Giovanni BOTTARI, Céline DE NADAI, Jukka-Pekka JALKANEN, François KAJZAR, David A. Leigh, Monika LUBOMSKA, Sandra M. MENDOZA, Jacek NIZIOL, Petra Rudolf, Francesco ZERBETTO

Research output: Contribution to journalArticle

Abstract

Surface enhanced second harmonic generation (SE SHG) experiments on molecular structures, macrocycles, catenanes, and rotaxanes, deposited as monolayers and multilayers by vacuum sublimation on silver, are reported. The measurements show that the molecules form ordered thin films, where the highest degree of order is observed in the case of macrocycle monolayers and the lowest in the case of rotaxane multilayers. The second harmonic generation activity is interpreted in terms of electric field induced second harmonic (EFISH) generation where the electric field is created by the substrate silver atoms. The measured second order nonlinear optical susceptibility for a rotaxane thin film is compared with that obtained by considering only EFISH contribution to SHG intensity. The electric field on the surface of a silver layer is calculated by using the Delphi4 program for structures obtained with TINKER molecular mechanics/dynamics simulations. An excellent agreement is observed between the calculated and the measured SHG susceptibilities.
Original languageEnglish
Pages (from-to)7648-7652
Number of pages5
JournalThe Journal of Physical Chemistry B
Volume110
Issue number15
DOIs
Publication statusPublished - 2006

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