Unusual and tunable one-photon nonlinearity in gold-dye plexcitonic Fano systems

Nano Letters
Fan NanZhenyu Zhang

Abstract

Recent studies of the coupling between the plasmonic excitations of metallic nanostructures with the excitonic excitations of molecular species have revealed a rich variety of emergent phenomena known as plexcitonics. Here, we use a combined experimental and theoretical approach to demonstrate new and intriguing aspects in the ultrafast nonlinear responses of strongly coupled hybrid Fano systems consisting of gold nanorods decorated with near-infrared dye molecules. We show that the severely suppressed linear absorption around the Fano dip significantly enhances the unidirectional energy transfer from the plasmons to the excitons and further allows one-photon nonlinearity to be drastically and reversibly tuned. These striking observations are interpreted within a microscopic model stressing on two competing processes: saturated plasmonic absorption and weakened destructive Fano interference from the bleached excitonic absorption. The unusually strong one-photon nonlinearity revealed here provides a promising strategy in fabricating nanoplasmonic devices with both pronounced nonlinearities and good figures of merit.

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Citations

Oct 5, 2016·Nano Letters·Hao WangShaozhi Deng
Feb 6, 2016·Chemical Society Reviews·Natalie L GruenkeRichard P Van Duyne
Aug 3, 2016·Nanoscale·Fan NanQu-Quan Wang
Jul 12, 2018·Nano Letters·Yuriy ZakharkoJana Zaumseil
Mar 17, 2018·The Journal of Physical Chemistry Letters·Gary BeaneGregory V Hartland
Sep 28, 2021·Chemical Reviews·Jiapeng ZhengJianfang Wang

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