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Effect of the Interface in Plasmon-enhanced Second Harmonic Generation from Nonlinear Optical Thin Films

Published online by Cambridge University Press:  17 April 2019

Hans D. Robinson
Affiliation:
Department of Physics, Virginia Tech, Blacksburg, VA, 24060
Kai Chen
Affiliation:
Department of Physics, Virginia Tech, Blacksburg, VA, 24060
Cemil Durak
Affiliation:
Department of Physics, Virginia Tech, Blacksburg, VA, 24060
Akhilesh Garg
Affiliation:
Department of Chemical Engineering, Virginia Tech, Blacksburg, VA, 24060
Richey M. Davis
Affiliation:
Department of Chemical Engineering, Virginia Tech, Blacksburg, VA, 24060
James R. Heflin
Affiliation:
Department of Physics, Virginia Tech, Blacksburg, VA, 24060
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Abstract

The second order nonlinear optical (NLO) properties of two different ionic selfassembled multilayer (ISAM) films combined with Ag nanoparticles have been investigated. The plasmon resonances in the Ag particles concentrate the incident light, markedly increasing in the NLO efficiencies of the films. We find that the efficiency enhancement is significantly larger in conventional ISAM films compared to films made using a hybrid covalent ISAM technique (HCISAM), even though the intrinsic bulk second order non-linear susceptibility (χ(2)) is much larger for HCISAM films. We attribute this to the interfaces in HCISAM films being much easier to disrupt by external perturbations such as the metal deposition by which the nanoparticles are fabricated. We conclude that because the plasmon decay length is very short, the plasmonic enhancement of NLO effects primarily occurs at and near the film-particle interface. To discern the importance of the interfaces, we surrounded thin ISAM and HCISAM films with NLOinactive buffer layers, which confirmed this hypothesis, particularly in the case of HCISAM films.

Type
Research Article
Copyright
Copyright © Materials Research Society 2010

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