Browsing by Subject "metal nanostructures"

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Open Access
Cascading and modifying nonradiative energy transfer mechanisms in strong coupling region of plasmons and excitons in semiconductor quantum dots
(2010) Akın, Onur
Nonradiative energy transfer finds important applications in nanophotonics and nanobiotechnology including nanoscale optical waveguiding and biological nanosensors. Various fluorophores can take part in such energy transfer interactions in close proximity of each other. Their emission kinetics can be strongly modified and controlled as a result. For example, colloidal semiconductor quantum dots, also known as nanocrystals, have widely been shown to serve as donors and acceptors among themselves or with other fluorescent species to transfer excitation energy nonradiatively. In their close proximity, emission characteristics of such fluorophores can also be altered when coupled with plasmonic structures, e.g., metal nanoparticles. One favored result of these plasmon-exciton interactions is the emission enhancement. In principle it is possible to plasmon-couple acceptor-donor pairs of nonradiative energy transfer to modify their transfer rate. Such plasmon-mediated energy transfer has been demonstrated, where both acceptor-donor pairs are plasmoncoupled. In these cases, however, the resulting plasmon-exciton interactions are not controlled to take place either at the donor site or the acceptor site but at both of the sites. Therefore, it has previously not been possible to identify the coupled interactions. In this thesis, we propose and demonstrate cascaded plasmonic - nonradiative energy transfer interactions that are controlled by selectively plasmon-coupling either only the donor quantum dots or only the acceptor quantum dots. For that, we designed a novel self-assembly architecture of our hybrid layered systems of semiconductor nanocrystals and metal nanoparticles in a bottom-up fashion through precise spatial and spectral control. This scheme uniquely allowed for the ability to spatially control plasmonexciton interactions to take place either at the “start” site (donors) or “finish” site (acceptors) of the energy transfer. This control was achieved by placing the plasmonic layer in the right proximity of the donors (for strong donor-exciton plasmon-coupling) while sufficiently being far away from the acceptors (for weak acceptor-exciton plasmon-coupling), or vice versa. Here we comparatively studied and analyzed consequent modifications of quantum dot emission kinetics in response to both cases of plasmon-coupling to only the donors and to only the acceptors through steady-state and time-resolved photoluminescence measurements, along with their lifetime and rate calculations. Such cascaded energy transfer interactions in the strong exciton-plasmon coupling region hold great promise for innovative near-field photonic devices and biological tags. system.
Open Access
Selective plasmonic control of excitons and their non-radiative energy transfer in colloidal semiconductor quantum dot solids
(2009) Özel, Tuncay
To date extensive research has proved that semiconductors and metals exhibit extraordinary optical properties in nano-dimensions compared to their bulk counterparts. For example, an interesting effect is observed in metal nanostructures/nanoparticles (NPs) that we form to obtain localized plasmons, with their optical response highly tuneable using the size effect. Another field of interest at the nanoscale is the investigation of light generation and harvesting using colloidal semiconductor quantum dot nanocrystals (NCs) that we synthesize in few nanometers, with their emission and absorption excitonic peaks conveniently tuneable using the size effect. In this thesis, we proposed and demonstrated the first accounts of selectively plasmonically-controlled colloidal quantum dot emitters assembled in innovative architectures, with a control achieved either through spatial selection or spectral selection. In the first set of designs, we developed for the first time plasmonic NC-composites that rely on spatially-selected plasmon-coupled CdTe NC-monolayers interspaced with respect to Au NP-monolayers in a repeating three-dimensional layer-by-layer architecture. In these bottom-up designs of hybrid nanocomposites, the photoluminescence kinetics is strongly modified and a record quantum efficiency of 30% is achieved for such CdTe NC solids. In the second set of designs, we showed the first spectrally-selected plasmon-coupling of surfaceemitting CdS NCs using optimized Ag NP deposits. This architecture allowed for the surface-state emission to be selectively enhanced while the interband emission is simultaneously suppressed in the same plasmon-coupled NCs, leading to the strongest surface-state emission from such CdS NCs reported with respect to their interband emission (with a >12-fold enhancement). Yet another important proximity phenomenon effective among quantum dot emitters is the Förster-type non-radiative resonance energy transfer (ET), in which excitonic excitation energy of the donor-NCs is non-radiatively transferred to the acceptor-NCs via dipole-dipole coupling. In the third set of our designs, we combined two fundamental proximity mechanisms of plasmon coupling and non-radiative energy transfer in the same NC solids. In plasmonic ET, we reported for the first time selectively plasmon-coupling of NC-acceptors and then that of NC-donors in the ET pair, both of which result in substantial enhancement of the acceptor emission with respect to ET with no plasmon coupling (with a maximum of 2-fold enhancement) as verified by their steadystate and time-resolved photoluminescence. This concept of spectrally/spatiallyselective plasmon coupling in quantum dots paves a new path for devices and sensors in nanophotonics.