Metallic nanostructures for enhanced sensing and spectroscopy




Ahmed, Aftab

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The interaction of light and matter at nanoscale is the subject of study of this dissertation. Particularly, the coupling of light to surface plasmons and their applications in the fields of spectroscopy and sensing is the focus of this work. In terms of spectroscopy, the simple reason of using light to study the chemical structures of different materials is the fact that the energy of light lies in the range of vibrational and electronic transitions of matter. Further, the ability to squeeze light to subwavelength dimensions opens up new possibilities of designing nano-optical devices. In this work we explore surface plasmons for two major applications: (i) Directivity enhanced Raman spectroscopy and (ii) Chemical/biological sensing. Here a new enhancement phenomenon has been demonstrated experimentally in regards to Raman spectroscopy. Typically, Raman enhancement is considered in terms of local fields only. Here we show the use of directive nanoantennas to provide additional enhancement of two orders of magnitude. The nanoantenna design is optimal in the sense that almost all of the scattered light is coupled into the numerical aperture of the collecting lens. It is shown that the additional enhancement from directivity pushes the sensitivity to single molecule regime. Further, the out of plane radiation and simplicity of the design makes it an ideal candidate for use with typical commercial microscope setups. Extra ordinary transmission through nanohole arrays in metallic films is studied for refractive index sensing. Bulk resolution of 6×10-7 is demonstrated by optimizing array dimensions, wavelength of operation, noise reduction and consideration of sensitivity of the detecting CCD camera. Self-assembled nanostructures are investigated for spectroscopic applications. Time dependent studies of nanorods assembled in end-to-end and side-by-side configurations are conducted. The end-to-end configuration results in higher local field enhancements whereas; the side-by-side configuration shows a reduction in local fields because of the cancellation of radial field components between the neighbouring nanorods. It should be noted that higher fields are desirable for Raman spectroscopy. Grating structures have been analysed using reduced coupled mode theory. In most cases, only three lowest order modes prove to be sufficient for accurate description of the system response. Here we present design guidelines for broadband operation and optimization of high quality factor resonators. Finally the complex reflection coefficient from arbitrary terminated nanorods has been investigated. Phase of reflection plays an important role in the determination of resonance wavelength of nanoantennas. It is shown that the localized surface plasmon resonance of nanoparticles can be considered in terms of propagating surface plasmons along a nanorod of similar geometry where the length of the nanorod approaches zero accompanied with π degrees of phase of reflection. The contributions made in this work can prove useful in the fields of analytical chemistry and biomedical sensing. The directive nanoantenna can find applications in a number of areas such as light emitting devices, photovoltaics, single photon sources and high resolution microscopy. Our work related to EOT based sensing is already approaching the resolution of commercially available refractive index sensors with the added advantage of multiplexed detection.



Nanoantenna, Raman Spectroscopy, Finite Difference Time Domain, Surface Plasmons, Sensing, Coupled Mode Theory, Nanohole Arrays, High Index Contrast Gratings, Self Assembly of Nano Rods