Plasmon-Exciton Resonant Energy Transfer: Across Scales Hybrid Systems

The presence of an excitonic element in close proximity of a plasmonic nanostructure, under certain conditions, may lead to a nonradiative resonant energy transfer known as Exciton Plasmon Resonant Energy Transfer (EPRET) process. The exciton-plasmon coupling and dynamics have been intensely studied in the last decade; still many relevant aspects need more in-depth studies. Understanding such phenomenon is not only important from fundamental viewpoint, but also essential to unlock many promising applications. In this review we investigate the plasmon-exciton resonant energy transfer in different hybrid systems at the nano- and mesoscales, in order to gain further understanding of such processes across scales and pave the way towards active plasmonic devices

Mechanism of emitters coupled with a polymer-based hyperbolic metamaterial

We study a polymer-based hyperbolic metamaterial (HMM) structure composed of three Au-polymer bilayers with a hyperbolic dispersion relation. Using an effective refractive index retrieval algorithm, we obtain the effective permittivity of the experimentally fabricated polymer-based structure. In particular, the unique polymer-based HMM shows the existence of high-k modes that propagate in the metal-dielectric multilayered structure due to the excitation of bulk plasmon-polaritonic modes. Moreover, we compare the experimental luminescence and fluorescence lifetime results of the multilayered Au and a dye-doped polymer (PMMA) to investigate the dynamics of three different emitters, each incorporated within the unique polymer-based HMM structure. With emitters closer to the epsilon-near-zero region of the HMM, we observed a relatively high shortening of the average lifetime as compared to other emitters either close or far from the epsilon-near-zero region. This served as evidence of coupling between the emitters and the HMM as well as confirmed the increase in the non-radiative recombination rate of the different emitters. We also show that the metallic losses of a passive polymer-based HMM can be greatly compensated by a gain material with an emission wavelength close to the epsilon-near-zero region of the HMM. These results demonstrate the unique potential of an active polymer-based hyperbolic metamaterial in loss compensation, quantum applications, and sub-wavelength imaging techniques.publishedVersionPeer reviewe

Graphene-based tunable plasmon induced transparency in gold strips

Plasmon induced transparency (PIT) has been numerically investigated and experimentally realized by two parallel gold strips on graphene for the mid-infrared (MIR) range. The PIT response is realized by the weak hybridization of two bright modes of the gold strips. The response of the device is adjusted with the lengths of two strips and tuned electrically in real time by changing the Fermi level (Ef) of the graphene. Ef is changed to tune the resonance frequency of the transparency window. A top gating is used to achieve high tunability and a 263 nm shift is obtained by changing the gate voltage from -0.6 V to 2.4 V. The spectral contrast ratio of our devices is up to 82%. (C) 2018 Optical Society of America under the terms of the OSA Open Access Publishing Agreement.publishedVersionPeer reviewe

Absorpitive losses mitigation in gain-plasmon hybrid systems as optical metamaterials

Scuola di Scienza e Tecnica "Bernardino Telesio", Dottorato di Ricerca in Scienza e Tecnologia delle Mesofasi e Materiali Molecolari, Ciclo XXVI, a.a.2013In the past decade, plasmonic nanoparticles (NPs) have gained a lot of interest due to their exceptional and fascinating properties which have been accomplishing vital role in emerging science and technology towards multifunctional applications. The extensive current research efforts in nanoplasmonics trigger towards various opto-electronic and medical applications such as invisibility, perfect lens, increasing the efficiency of solar cells, designing and extra-sensitive single-particle detection of biomolecular recognition and in particular optical metamaterials. The negative real part and the low value of the imaginary part of dielectric permittivity are crucial for applications of nanoparticles as subunits of optical metamaterials. However, the performance of plasmonic nanostructures is significantly limited by the intrinsic and strong energy dissipation in metals, especially in the visible range. In fact, regardless of the challenges to synthesize plasmonic nanostructures, the path to use them as building blocks of optical metamaterial is crossing through the finding a solution to mitigate their optical losses. In this research thesis, it is demonstrated experimentally that the incorporation of gain material such as organic dye molecules and quantum dots in close proximity of enhanced local fields of various properly designed plasmonic systems makes it possible to induce resonant energy transfer processes from gain units to plasmonic nanoparticles, to accompanish loss compensation in optical metamaterials. Steady-state experiments and time resolved spectroscopy along with modification of Rayleigh scattering and optical transmission of a probe beam as a function of impinging energy are crucial evidences of mitigation of absorptive losses in different gain doped plasmonic systems The strategy that has been followed here towards mitigation of absorptive losses in optical metamaterials acts at different spatial scales from nano to macro (see Figure 1). The systems at nano-scale (10-100 nm) are based on dispersion of NPs, in particular, gain assisted (nanoparticle-dye dispersion), gain-functionalized core-shell gold NPs (encapsulated dye molecules into the shell) and dye grafted gold core multimeric nanostructures. The study of such nano-composites allows to recognize experimentally how the parameters such as the geometry and size of the metal nanostructures, inter-particle distance, overlap between emission spectrum of gain material and plasmon band of metal NPs, concentration and quantum yield of donor molecules are playing an important role to create more efficient nonradiative RET processes from donor molecules to acceptors. Figure 1 The followed spatial stages on this research study ranged from (a) nano-scale and (b) mesco scale towards (c) macro scale. The obtained results in nano-scale generate further motivations to move forward to study meso-scale (100-900 nm) plasmonic systems which include both dispersion (nanoshell composites) and bulk (periodic layers of gain materials and lossy metal elements) systems. The nanoshells which are consisted of dye doped dielectric core coated gold shell dispersed in ethanol solution are designed with an optimized ratio of core diameter and metallic shell thickness. The time resolved fluorescence spectroscopy results along with pump-probe experiments on nanoshells are convincing evidences for optical loss mitigation. Finally in third stage, the optical properties of gain-plasmon composites dispersed in PDMS host matrix as an example for bulk samples at the macroscopic scale (1 μm and beyond) have been investigated. The achieved results on this stage can help to design and fabricate such plasmonic structures that lead from fundamental physics towards practical applications. In this regard, the first four chapters provide the background concerning the main elements of this research work. The first chapter contains an introduction to the metamaterials. Second chapter describes the optical properties of plasmonic nanostructures. In third chapter, gain materials and the optical processes beyond these materials have been investigated. The fourth chapter deals with the optical properties of hybrid systems consisted of active materials and nano-plasmonic elements. After providing a brief introduction regarding the applied setups and instruments in this research study in chapter five, the last three chapters represent the acquired experimental results in each mentioned spatial scale. In chapter six, the optical properties of nano-scaled gain-plasmon systems in solution including gain-assisted, gainfunctionalized and dye grafted multimeric samples are investigated. Chapter seven explores the optical characteristics of dispersion of nanoshell sample as an example of the study in mesoscale. Finally, the thesis is completed with the study of the optical features of macro-scaled bulk samples based on core–shell type quantum dots and gold NPs dispersed in PDMS, and a short conclusion of this research study. This study emphasizes effective progress in materials science and paves the way towards further promising scientific research aimed to enable the wide range of electromagnetic properties of plasmonic metamaterialsUniversità della Calabri

Generation of additive colors with near unity amplitude using a multilayer tandem Fabry–Perot cavity

In this paper, the generation of additive red-green-blue (RGB) colors in reflectance mode with near unity amplitude is demonstrated. For this purpose, a multilayer structure made of metal–insulator–metal–semiconductor–insulator stacks is designed to achieve >0.9 reflection peaks with full-width-at-half-maximum values <0.3peak. The proposed design also shows near zero reflection in off-resonance spectral ranges, and this, in turn, leads to high color purity. The optimized designs are fabricated, and simulation and theoretical results are verified with characterization findings. This work demonstrates the potential of multilayer tandem cavity designs in the realization of lithography-free large-scale compatible functional optical coatings.acceptedVersionPeer reviewe

Battling absorptive losses by plasmon-exciton coupling in multimeric nanostructures

© The Royal Society of Chemistry 2015. The strong inherent optical losses present in plasmonic nanostructures significantly limit their technological applications at optical frequencies. Here, we report on the interplay between plasmons and excitons as a potential approach to selectively reduce ohmic losses. Samples were prepared by functionalizing plasmonic core-shell nanostructures with excitonic molecules embedded in silica shells and interlocked by silica spacers to investigate the role played by the plasmon-exciton elements separation. Results obtained for different silica spacer thicknesses are evaluated by comparing dispersions of plasmonic multimers with respect to the corresponding monomers. We have observed fluorophore emission quenching by means of steady-state fluorescence spectroscopy, as well as a significant shortening of the corresponding fluorescence lifetime using TCSPC data. These results are accompanied by the simultaneous enhancement of Rayleigh scattering and transmittance, revealing more effective absorptive loss mitigation for multimeric systems. Moreover, upon decreasing the thickness of the intermediate silica layer between gold cores and the external gain functionalized silica shell, the efficiency of exciton-plasmon resonant energy transfer (EPRET) was significantly enhanced in both multimeric and monomeric samples. Simulation data along with experimental results confirm that the hybridized plasmon fields of multimers lead to more efficient optical loss compensation with respect to the corresponding monomers