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Proceedings Paper

Observation of coherent optical coupling within inorganic-organic hybrid nanoparticles
Author(s): Gregory A. Wurtz; Jasmina Hranisavljevic; Gary P. Wiederrecht
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Paper Abstract

We report on the study of the optical properties of hybrid systems made from molecular aggregates (J-aggregates) and metallic nanoparticles (Au and Ag). Both entities have outstanding optical properties that have been extensively addressed both through experimental and theoretical efforts. The J-aggregates were chosen for their linear and non-linear excitonic response that shows among other intriguing properties, superradiant emission, ultrafast optical switching, and electroluminescence. These J-aggregates form spontaneously on the surface of Au and Ag nanoparticles, used primarily to excite the organic shell through optical near-field interaction. Steady state as well as ultrafast spectroscopic measurements was used to characterize the nature of the interaction between the two constituents as well as to follow the dynamics of the exciton in the aggregate upon near-field excitation from the particle. For both Au and Ag, Mie scattering theory calculations of the hybrid ground state absorption spectra account for the experimental observations and reflect the coherent coupling between the excitonic states in the aggregate and the nanoparticles electronic transition dipoles. Furthermore we show that the dipole-dipole coupling strength between the individual molecules in the aggregate is increased by ~30% on the surface of the particle compared to its value in solution. The different dynamics of these nanosystems have been probed using femtosecond spectroscopy and reveals contrasted relaxation pathways for the exciton when interacting with Ag with respect to Au as well as a delay dependent excitonic coherent length.

Paper Details

Date Published: 8 September 2004
PDF: 10 pages
Proc. SPIE 5464, Organic Optoelectronics and Photonics, (8 September 2004); doi: 10.1117/12.545684
Show Author Affiliations
Gregory A. Wurtz, Argonne National Lab. (United States)
Jasmina Hranisavljevic, Argonne National Lab. (United States)
Gary P. Wiederrecht, Argonne National Lab. (United States)

Published in SPIE Proceedings Vol. 5464:
Organic Optoelectronics and Photonics
Paul L. Heremans; Michele Muccini; Hans Hofstraat, Editor(s)

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