This thesis discusses the design and construction of a Near-field Scanning Optical Microscope (NSOM). Basic principles of operation, the characteristics of the hardware components, and the control software are discussed. A unique method of controlling the position of the probe is developed, and scans of a diffraction grating are presented. We show the influence that the surface topology and reflectivity and the interference of direct and reflected light have on the images. A second design of the instrument, for use in a vacuum chamber and with a flexure stage for lateral motion, is accomplished. / text

Surface Plasmon Polaritons (SPPs) are considered to be attractive components for plasmonics and nanophotonic devices due to their sensitivity to interface changes, and their ability to guide and confine light beyond the diffraction limit. They have been utilized in SPP resonance sensors and near field imaging techniques and, more recently, SPP experiments to monitor and control ultrafast charge carrier and energy relaxation dynamics in thin films. In this thesis, we discuss excitation and propagation properties of ultrafast SPPs on thin extended metal films and SPP waveguide structures. In addition, localized and propagating surface plasmon interactions in functional plasmonic nanostructures will also be addressed. For the excitation studies of ultrafast SPPs, we have done detailed analysis of femtosecond surface plasmon pulse generation under resonant excitation condition using prism coupling technique. Our results show that photon-SPP coupling is a resonant process with a finite spectral bandwidth that causes spectral phase shift and narrowing of the SPP pulse spectrum. Both effects result in temporal pulse broadening and, therefore, set a lower limit on the duration of ultrafast SPP pulses. These findings are necessary for the successful integration of plasmonic components into high-speed SPP circuits and time-resolved SPP sensors. To demonstrate interactions between localized and propagating surface plasmons, we used block-copolymer based self assembly techniques to deposit long range ordered gold nanoparticle arrays onto silver thin films to fabricate composite nanoparticle thin film structures. We demonstrate that these gold nanoparticle arrays interact with SPPs that propagate at the film/nanoparticle interface and therefore, modify the dispersion relation of SPPs and lead to strong field localizations. These results are important and advantageous for plasmonic device applications. For the propagation studies of ultrafast SPPs, we have designed and constructed a home-built femtosecond photon scanning tunneling microscope (fsPSTM) to visualize ultrafast SPPs in photonic devices based on metal nanostructures. Temporal and phase information have been obtained by incorporating the fsPSTM into one arm of a Mach-Zehnder interferometer, allowing heterodyne detection. Understanding plasmon propagation in metal nanostructures is a requirement for implementing such structures into opto-electronic and telecommunication technologies.

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La construction d’un NSOM, dans ce manuscrit de thèse, est décrite en détail. Lacombinaison du système NSOM construit avec un interféromètre est proposée afin d’accéderà des mesures de phase, à la fois de ultra-haute sensibilité mais également de très granderésolution spatiale. Le nom de l’instrument développé est un interferomètre optique àbalayage en champ proche (NSOI, pour l’acronyme en anglais). Le principe est basé surl’utilisation d’un diapason accordable en cristal de quartz, sur lequel se trouve une pointe,afin de sonder le matériau étudié. La mesure de la force de cisaillement de la pointe sondeau voisinage de la surface permet d’assurer la régulation et la stabilité de la distance depositionnement de la pointe par rapport à la surface considérée. Le dispositif est construit encombinant différents éléments électroniques pilotés par un logiciel développé en langageLab-VIEW. Le bruit de la mesure en NSOI est supprimé par un calcul simple basé sur lathéorie de l’optique ondulatoire et des interférences associées. Le système permet deréaliser des mesures optiques en champ proche ainsi que la détermination en hauterésolution de la phase du champ optique. L’échantillon SNG01 (l’un des réseaux utilisés pourcaractériser notre microscope à balayage en champ proche), ainsi que des disques optiques(CD, DVD and disques blu-ray) ont été utilisés pour tester la faisabilité et les performancesde notre système.Dans ce manuscrit de thèse, le graphène et les monocouches de MoS2 sont étudiés. Nous montrons qu’une épaisseur à l’échelle atomique peut être résolue par notresystème NSOI, avec l’utilisation de l’algorithme de suppression du bruit de mesure. Lesjoints de grain du graphène sont observés à grande échelle, via la technique d’imagerie parcollection en champ proche et par la réalisation de cartographies de phase. En particulier,les tensions internes à une couche de graphène sont observées, uniquement dans le casd’une imagerie de phase. / In this thesis, near-field scanning optical interferometry (NSOI), which combinesNSOM with interferometer, is proposed for the phase measurement. The shear-forcedetection scheme is applied for distance regulation. The hardware of the systemis constructed by combining various electronic devices, and the operating softwareis coded by LabVIEW. Unwanted background signal is removed by simple calculationbased on interference theory. By using this, the near-field optical measurementand the ultra-sensitive phase investigation of nano-materials are performed. 2D materialssuch as graphene and monolayer MoS2 are investigated. It is shown thatatomic-scale thickness can be resolved by the NSOI. Especially, the grain boundariesof graphene and the seed of MoS2 can be found by phase detection. In addition,direct laser writing (DLW) on silver-containing glass is observed by using NSOM,and NSOI. For the first time, the writing threshold is correlatively observed in thefluorescence imaging and the near-field phase image.