Journal
JOURNAL OF PHYSICAL CHEMISTRY A
Volume 114, Issue 28, Pages 7590-7594Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jp102438m
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Funding
- office of Vice President for Research at the University at Buffalo
- National Science Foundation
- Swedish Infrastructure Committee (SNIC) [SNIC 022/09-25]
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We show that ultrasmall metallic nanoparticles can be combined with large second- and third-order response organic chromophores to enhance the overall third-order response of the system. This approach can be used in combination with microscopic cascading to generate exceptionally large third-order response. Intermolecular charge-transfer coupling between the molecules and the metal clusters enhances the real part of the nonlinearity at telecommunication wavelengths, while avoiding plasmonic enhancement of one- and two-photon absorption, and minimizing optical losses. The results of density functional calculations for a molecule with large second-order response, (para)nitroaniline, show that use of a gold cluster as a link between molecular entities enhances third-order nonlinearity. Varying size and shape of the metal cluster as well as the distance between the clusters and the molecules allows fine-tuning of nonlinear response over a large range of magnitudes.
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