Browsing by Subject "plasmonic nanostructures"

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Open Access
Novel light-sensitive nanocrystal skins
(2013) Akhavan, Shahab
Light sensing devices traditionally made from crystalline or amorphous silicon, operating at the visible and near-infrared wavelengths, have led to a multibillion-dollar annual market. However, silicon faces various limitations including weak detection at long wavelengths (insufficient beyond 1.1 µm) with a cut-off at short wavelengths (in the ultraviolet) and small-area applications. On the other hand, solution-processed semiconductor nanocrystals (NCs), also known as colloidal quantum dots, offer large-area light sensing platforms with strong absorption cross-section. In this thesis we propose and demonstrate a new class of large-area, semi-transparent, light-sensitive nanocrystal skin (LS-NS) devices intended for large-surface applications including smart transparent windows and light-sensitive glass facades of smart buildings. These LS-NS platforms, which are fabricated over areas up to many tens of cm2 using spraycoating and several cm-squares using dip-coating, are operated on the basis of photogenerated potential buildup, as opposed to conventional charge collection. The close interaction of the monolayer NCs of the LS-NS with the top interfacing metal contact results in highly sensitive photodetection in the absence of external bias, while the bottom side is isolated using a high dielectric spacing layer. In operation, electron-hole pairs created in the NCs of the LS-NS are disassociated and separated at the NC monolayer - metal interface due to the difference in the workfunctions. As a result, the proposed LS-NS platforms perform as highly sensitive photosensors, despite using a single NC monolayer, which makes the device semi-transparent and reduces the noise generation Furthermore, because of the band gap tunability, it is possible to construct cascaded NC layers with a designed band gap gradient where the NC diameters monotonically change. Here we present the first account of exciton funneling in an active device, which leads to significant performance improvement in the device. We show highly photosensitive NC skins employing the exciton funneling across the multiple layers of NC film. To further enhance the device photosensitivity performance, we demonstrate embedding plasmonic nanoparticles into the light-sensitive skins of the NCs. In addition, we exhibit the LS-NS device sensitivity enhancement utilizing the device architecture of semi-transparent tandem skins, the addition of TiO2 layer for increased charge carrier dissociation, and the phenomenon of multiexciton generation in infrared NCs. With fully sealed NC monolayers, LS-NS is found to be highly stable under ambient conditions, promising for low-cost large-area UV/visible sensing in windows and facades of smart buildings. We believe the findings presented in this thesis have significant implications for the future design of photosensing platforms and for moving toward next generation large-surface light-sensing platforms.
Open Access
Three dimensional nanoplasmonic surfaces : modeling, fabrication and characterization
(2013) Güngör, Kıvanç
Today designing functional nanoplasmonic structures specific to a variety of applications attracts great interest from various fields ranging from optoelectronics to life sciences. There are numerous ways of making nanoplasmonic structures. Among them, nanopatterning of a thin-film metal layer is one of the most common approaches, which allows for finely controlled fabrication of a plasmonic unit and their repeating layout in the plane of the starting metal film. Although there are many examples of such nanopatterned plasmonic structures reported to date, they are typically designed and implemented on a planar surface. In these architectures, plasmonic layout commonly covers significantly less than 100% of the substrate surface and can provide field localization most strongly around the sharp corners and small gaps between the patterns. In the case of using a periodic layout, which is commonly employed for experimental realization (although periodicity is not necessary), the plasmonic array inherently yields a duty cycle substantially less than unity (usually close to 0.5). As a result, the surface coverage of nanopatterned plasmonic structures on a planar surface has intrinsically been limited and the field enhancement across their nanoplasmonic layout has been possible mostly in the plane and slightly above it. To address these limitations, this thesis proposed and demonstrated three-dimensional (3D) nanoplasmonic arrayed structures designed and implemented on a non-planar surface that allows for strong field enhancement in the out-of-plane direction and enables a very large surface coverage of the substrate close to unity. The thesis work included both numerical modeling and experimental characterizations. As a proof-of-concept demonstration, we fabricated non-planar arrays of checkerboard nanostructures, each with two-fold rotational symmetry, laid out in a volumetric fashion as two interlocked square lattice arrays at two different levels, facilitating strong field localization vertically between these two complementary planes. The resulting nanofabricated samples exhibited a maximum surface coverage of 100% in plan view. With full electromagnetic solution of such 3D nanoplasmonic surfaces, we showed that the out-of-plane field localization is 7.2-fold stronger than the inplane localization, in comparison to their two-dimensional (2D) components alone. These numerical results agree well with the experimental observations including far-field optical transmission and reflection measurements. The absorption spectroscopy further revealed that the resulting spectrum of the 3D checkerboard features a unique signature arising from the out-of-plane localization, which does not exist in the case of the 2D counterparts. These results indicate that 3D nanoplasmonics of such non-planar surfaces provides us with the ability to generate and better utilize the plasmonic volume, possibly useful for increased plasmonic coupling and interactions.