Nanoscale lithography is the key component of the semiconductor device fabrication process. For the sub-10 nm node device, the conventional deep ultraviolet (DUV) photolithography approach is limited by the diffraction nature of light even with the help of double or multiple patterning. The upcoming extreme ultraviolet (EUV) photolithography can overcome this resolution limit by using very short wavelength (13.5nm) light. Because of the prohibitive cost of the tool and the photomask, the EUV lithography is only suitable for high volume manufacturing of high value. Several alternative lithography technologies are proposed to address the cost issue of EUV such as directed self-assembly (DSA), nanoimprint lithography (NIL), scanning probe lithography, maskless plasmonic photolithography, optical maskless lithography, multiple electron-beam lithography, etc.<div><br></div><div>Electron-beam lithography (EBL) utilizes a focused electron beam to write patterns dot by dot on the silicon wafer. The beam size can be sub-nanometers and the resolution is limited by the resist not the beam size. However, the major drawback of EBL is its low throughput. The throughput can be increased by using large current but at the cost of large beam size. This is because the interaction between electrons in the pathway of the electron beam. To address the trade-off between resolution and throughput of EBL, the multiple electron-beam lithography was proposed to use an array of electron-beams. Each beam has a not very large beam current to maintain good resolution but the total current can be very high to improve the throughput. One of the major challenges is how to create a uniform array of electron beamlets with large brightness.<br></div><div><br></div><div>This dissertation shows a novel low-cost high-throughput multiple electron-beam lithography approach that uses plasmonic enhanced photoemission beamlets as the electron beam source. This technology uses a novel device to excite and focus surface electromagnetic and electron waves to generate millions of parallel electron beamlets from photoemission. The device consists of an array of plasmonic lenses which generate electrons and electrostatic micro-lenses which guide the electrons and focus them into beams. Each of the electron beamlets can be independently controlled. During lithography, a fast spatial optical modulator will dynamically project light onto the plasmonic lenses individually to control the switching and brightness of electron beamlets without the need of a complicated beamlet-blanking array and addressable circuits. The incident photons are first converted into surface electromagnetic and electron waves by plasmonic lens and then concentrated into a diffraction-unlimited spot to excite the local electrons above their vacuum levels. Meanwhile, the electrostatic micro-lens will extract the excited electrons to form a finely focused beamlet, which can be rastered across a wafer to perform lithography. The scalable plasmonic enhanced photoemission electron-beam sources are designed and fabricated. An array of micro-scale electrostatic electron lenses are designed and fabricated using typical micro-electro-mechanical system (MEMS) fabrication method. The working distance (WD) defined as the gap from the electron lens to the underneath silicon wafer is regulated using a gap control system. A vacuum system is designed and constructed to host the multiple electron-beam system. Using this demo system, the resolution of the electron beams is confirmed to be better than 30 nm from the lithography results done on poly methyl methacrylate (PMMA) and hydrogen silsesquioxane (HSQ) resists. According to simulation results, the electron beam spot size can be further optimized to be better than 10 nm.<br></div><div><br></div><div>This scheme of high-throughput electron-beam lithography with multiple plasmonic enhanced photoemission beamlets has the potential to be an alternative approach for the sub-10 nm node lithography. Because of its maskless nature, it is cost effective and especially suitable for low volume manufacturing and prototype demonstration.<br></div><div><br></div><div><br></div>

The subject of this thesis is the investigation of organic microcavities with implemented unstructured and laterally structured metal layers. The optical properties are studied by means of various spectroscopic techniques and are compared to conventional metal-free devices. It is shown that the large expected absorption caused by the embedded metal is reduced compared to the case of a free-standing metal layer of the same thickness. As a consequence of the interaction of the photonic cavity mode with the metallic structures, two new coupled modes emerge which are called Tamm plasmons. The strength of this coupling and the resulting spectral difference of these modes are defined by the thickness of both the metal layer and the adjacent dielectric layers. These control parameters enable the optimization of the structural design. Accordingly, coherent emission from Tamm plasmons is realized at room temperature. An analytical approach is developed accounting for the experimentally observed polarization splitting of detuned resonances. Next, laterally structured metal layers embedded into organic microcavities are considered. The structuring leads to a confinement of the photonic density of states evident from a clear discretization in energy of the corresponding modes. Applying a photolithographic technique to structure the metal layer into a pattern of regularly placed stripes leads to additional effects due to the resulting periodicity. By exciting this hybrid structure above a certain threshold, periodic arrays of localized cavity modes and metal-based Tamm plasmons are generated. These Bloch-like excited states are capable of phase coupling across the grating. Additionally, surface plasmon polaritons (SPPs) are excited propagating at the interface of the silver and the adjacent dielectric layers. Thanks to the periodicity of the metallic stripes, SPPs are subject to efficient Bragg scattering into the light cone in air. Modes up to order number 30 are detectable as quasi-linear periodic lines in the dispersion pattern. A Fourier analysis reveals an in- or out-of-phase coupling of the modes and a spread of the coherence over macroscopic distances of more than 40 µm. This strategy of embedding metal patterns into an organic microcavity yields a viable route towards electrically contacted organic solid-state lasers. / In dieser Arbeit werden erstmals dünne, unstrukturierte sowie lateral strukturierte metallische Schichten in organische Mikroresonatoren eingebettet und anschließend die optischen Eigenschaften mittels spektroskopischer Verfahren untersucht. Es zeigt sich, dass die erwarteten hohen optischen Verluste durch die Absorption des elektrischen Feldes im Metall deutlich reduziert sind, verglichen mit dem Fall einer freistehenden, nicht eingebetteten Metallschicht gleicher Dicke. Als Folge der Wechselwirkung der photonischen Kavitätsmode mit dem Metall spaltet diese in zwei miteinander gekoppelte Moden auf. Diese neuartigen Moden werden als Tamm-Plasmonen bezeichnet. Die Kopplung sowie die spektrale Differenz beider Moden ist zum einen durch die optischen Eigenschaften und die Dicke der eingebetteten Metallschicht definiert, zum anderen durch die optische Dicke der angrenzenden dielektrischen Schichten. Dadurch ist eine Optimierung des Systems im Hinblick auf Absorption und Emissionswellenlänge der Bauteile möglich, so dass selbst bei Raumtemperatur kohärente Emission eines Tamm-Zustands erzielt werden kann. Eine erarbeitete analytische Rechnung bestätigt und erklärt die experimentell gemessene, polarisationsabhängige Aufspaltung der auftretenden resonanten Moden. Im zweiten Teil der Arbeit sind organische Mikroresonatoren, deren eingebettete Metallschicht in lateraler Richtung auf verschiedene Weisen strukturiert sind, Gegenstand der Untersuchungen. Als Folge dieser Strukturierung kommt es zur lateralen Beschränkung der photonischen Zustandsdichte, was durch eine Diskretisierung der Energiespektren der resultierenden optischen Moden experimentell nachweisbar ist. Werden periodische Metallstreifen mittels Photolithographie erzeugt, so kommt es neben einer weiteren Beeinflussung der Zustandsdichte auch zu Effekten, die durch diese Periodizität bedingt sind. Entsprechend reproduziert sich die Kavitätsmode mehrfach im Impulsraum. Oberflächenplasmonen, die auf der Grenzfläche zwischen dem Metall und den dielektrischen Schichten propagieren, werden auf Grund der Periodizität bis in den experimentell zugänglichen Lichtkegel gestreut. Dabei werden Plasmonenresonanzen bis hin zur 30. Ordnung gemessen. Im letzten Experiment werden derart periodisch strukturierte Metall-Organik-Mikroresonatoren auf ihre Lasertätigkeit hin untersucht. Eine lokal begrenzte optische Anregung mittels eines gepulsten Lasers führt zur Ausbildung verschiedener Bloch-ähnlicher Moden, deren Kohärenz sich lateral bis zu 40 µm ausbreitet. Eine Fourieranalyse zeigt eindeutige und feste Phasenbeziehungen zwischen angrenzenden Maxima der Moden. Zusammenfassend ergeben sich interessante metall-organische Systeme, die minimale Absorption und niedrige Laserschwellen aufweisen und die prinzipielle Eignung zur elektrischen Kontaktierung besitzen.

Tato diplomová práce se zabývala plazmonickými anténami pro infračervenou oblast spektra elektromagnetického záření. K hledání zesílení pole bylo použito FDTD (Finite-Difference Time-Domain Method) simulací. Podle očekávání, byla shledána lineární závislost rezonanční vlnové délky na délce raménka platinové antény na křemíkovém povrchu. Diplomová práce se také zabývala výrobou antén pomocí fokusovaného iontového svazku (FIB) a následným měřením rezonančních vlastností pomocí mikroskopické metody FT-IR (Fourier Transform Infrared Spectroscopy). Posun rezonanční vlnové délky byla registrována pouze pro negativní antény. Nakonec se tato práce zabývala vysvětlením saturace křivky závislosti rezonanční vlnové délky na rozměru raménka platinové antény na substrátu ze SRONu (silicon-rich oxynitride).

Práce pojednává o vlastnostech plazmonických antén v infračervené a viditelné oblasti. Práce zahrnuje výrobu, měření a numerické modelování optických vlastností antén. Infračervené plazmonické antény na absorbujícím substrátu (SRON) jsou studovány pro jejich rezonanční a absorpční vlastnosti. Byla nalezena geometrie antény, která poskytuje maximální účinnost absorpce ve SRON vrstvě. Dále je studována možnost zesílení daného vibračního módu substrátu (obsahujícího 3-4 materiálové rezonance) pomocí plazmonické rezonance antény. Nakonec jsou prezentována měření katodoluminiscenčních spekter antén ve viditelném spektru.

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This dissertation provides what the author believes to be perhaps the first experimental evidence of single electrons passing both ends of a suspended split-ring resonator, with many applications for future nanophotonic devices, and novel implications for research into surface plasmons. / Swift electrons passing near metal-dielectric interfaces can excite travelling electromagnetic waves confined to the charge density at the interface, known as surface plasmon polaritons (SPPs). The excitation process retards the swift electrons to an extent which can be resolved using electron energy loss spectroscopy (EELS). Scanning transmission electron microscopy (STEM) paired with EELS can characterize these losses with high energy and spatial resolution but is a time-averaged technique. Hence, spectral data provides statistical information about the number of electrons which underwent a particular energy exchange, but their existences are otherwise spatiotemporally ambiguous. We have developed and tested a scheme which partially lifts this veil. This thesis details the steps taken to fabricate a split-ring resonator so that single electrons sequentially pass by both ends of the resonator, enabling what we refer to here as double-pass EELS. We provide evidence that single electrons have excited SPPs in both events, and that this aloof analogue to common plural scattering may also lead to an amplification in the second event. This suggests that our technique could be considered a single electron pump-probe spectroscopy, with wide-ranging applications, particularly in quantum research. / Dissertation / Doctor of Philosophy (PhD) / The future of computing may reside in a foundation of quantum technologies, where circuits which use light instead of electrical currents hold much promise. However, minimization of photonic (i.e. light based) components is limited by diffraction; we cannot guide light through channels that have arbitrarily small widths. We can exceed this limit by coupling the light into a ripple in the sea of electrons at the surface of a metal. These are known as surface plasmon polaritons, which can be confined to scales much smaller than what is accessible to light. Surface plasmon polaritons can alternatively be initiated when fast electrons pass by the metal surface and generate tides in the sea of electrons. The electrons lose a measurable amount of energy in this interaction which we can track to study the surface plasmon polaritons. I have worked with staff at the Canadian Centre for Electron Microscopy to design and fabricate U-shaped structures which have allowed a new class of experiments in which a single fast electron can pass by both ends, one after the other. This thesis explains the observed signatures in the energies of the collected electrons, including evidence that single electrons can excite two separate surface plasmon polaritons with a designed delay of around ten millionths of a billionth (10^-14) of a second. We also discuss the implications of these experiments for a wide range of potential applications. Additional works herein include simulations of the entanglement between fast electrons and surface plasmons, and analysis of spectral properties for ensembles of gold and silicon nanoparticles, given that the split-ring resonators are primarily made from those materials. Ultimately, this work introduces a new domain of possible experiments for electron energy loss spectroscopy in which we can characterize some of the ultrafast dynamics of surface plasmon polaritons within a time-averaged technique.

We introduce an approach to implement full coherent control on nanometer length scales. It is based on spatiotemporal modulation of the surface plasmon polariton (SPP) fields at the thick edge of a nanowedge. The SPP wavepackets propagating toward the sharp edge of this nanowedge are compressed and adiabatically concentrated at a nanofocus, forming an ultrashort pulse of local fields. The profile of the focused waveform as a function of time and one spatial dimension is completely coherently controlled. We establish the principal limits for the nanoconcentration of the terahertz (THz) radiation in metal/dielectric waveguides and determine their optimum shapes required for this nanoconcentration. We predict that the adiabatic compression of THz radiation from the initial spot size of vacuum wavelength R λ 300 μm 0 0 ≈ ≈ to the unprecedented final size of R = 100 − 250 nm can be achieved, while the THz radiation intensity is increased by a factor of 10 to 250. This THz energy nanoconcentration will not only improve the spatial resolution and increase the signal/noise ratio for THz imaging and spectroscopy, but in combination with the recently developed sources of powerful THz pulses, will allow the observation of nonlinear THz effects and a variety of nonlinear spectroscopies (such as two-dimensional spectroscopy), which are highly informative. This should find a wide spectrum of applications in science, engineering, biomedical research and environmental monitoring. We also develop a theory of the spoof plasmons propagating at the interface between a dielectric and a real conductor. The deviation from a perfect conductor is introduced through a finite skin depth. The possibilities of guiding and focusing of spoof plasmons are considered. Geometrical parameters of the structure are found which provide a good guiding of such modes. Moreover, the limit on the concentration by means of planar spoof plasmons in case of non-ideal metal is established. These properties of spoof plasmons are of great interest for THz technology.

We introduce an approach to implement full coherent control on nanometer length scales. It is based on spatiotemporal modulation of the surface plasmon polariton (SPP) fields at the thick edge of a nanowedge. The SPP wavepackets propagating toward the sharp edge of this nanowedge are compressed and adiabatically concentrated at a nanofocus, forming an ultrashort pulse of local fields. The profile of the focused waveform as a function of time and one spatial dimension is completely coherently controlled. We establish the principal limits for the nanoconcentration of the terahertz (THz) radiation in metal/dielectric waveguides and determine their optimum shapes required for this nanoconcentration. We predict that the adiabatic compression of THz radiation from the initial spot size of vacuum wavelength ~300 μm to the unprecedented final size of 100-250 nm can be achieved, while the THz radiation intensity is increased by a factor of 10 to 250. This THz energy nanoconcentration will not only improve the spatial resolution and increase the signal/noise ratio for THz imaging and spectroscopy, but in combination with the recently developed sources of powerful THz pulses, will allow the observation of nonlinear THz effects and a variety of nonlinear spectroscopies (such as two-dimensional spectroscopy), which are highly informative. This should find a wide spectrum of applications in science, engineering, biomedical research and environmental monitoring. We also develop a theory of the spoof plasmons propagating at the interface between a dielectric and a real conductor. The deviation from a perfect conductor is introduced through a finite skin depth. The possibilities of guiding and focusing of spoof plasmons are considered. Geometrical parameters of the structure are found which provide a good guiding of such modes. Moreover, the limit on the concentration by means of planar spoof plasmons in case of non-ideal metal is established. These properties of spoof plasmons are of great interest for THz technology.

As visual display technologies move closer to producing true three dimensional displays, pixel technologies need to be ever smaller and more functional to keep pushing the boundaries. Plasmonic metasurfaces have been shown to control the phase, amplitude and/or polarisation of incoming electromagnetic radiation. Nano-fabrication advancements have resulted in the fabrication of the building blocks of such metasurfaces at nano-scale dimensions, allowing the surfaces to interact with visible light, opening up applications in visual displays. As pixel sizes shrink, smaller colour filters will be required. The excitation of plasmonic resonances in metallic nano-structure arrays have resulted in colour filters an order of magnitude smaller than what is currently commercially available. As colour filters, plasmonic metasurfaces offer numerous advantages over pigment-based colour filters used in modern commercial liquid crystal (LC) displays, including environmental, size and longevity factors. Furthermore, exploiting the wavelength and polarisation dependant scattering of nano-structures, optical components, including lenses, waveplates and holograms containing sub-wavelength pixels have been demonstrated in the visible wavelength spectrum. The metasurfaces are able to mould optical wavefronts into arbitrary shapes with sub-wavelength resolution by introducing spatial variations in the optical response of the light scatterers. The applications demonstrated so far are, on the whole, static devices, that is to say their optical properties may not be altered post fabrication. To realise the full potential of plasmonic metasurfaces to visual applications the devices must be made active. By activating structural colour surfaces, not only may pixel densities potentially be increased simply by removing the need for separate red, green and blue filters, but a new class of high definition ultra-thin display devices may be accessible, whilst the dynamic manipulation of the wavelength and polarisation properties of nano-scattering elements would open up the possibilities to create sub-wavelength holographic pixels. This thesis investigates ways to activate static metasurfaces for colour, flat optic, and holographic applications. First, methods of dynamic control of the structural colour of plasmonic nano-hole arrays are investigated. By combining nano-hole arrays with liquid crystals, transmissive electrically tunable LC-nanohole pixels operating across the visible spectrum with un-polarised input light are experimentally demonstrated. An output analyser in combination with a nematic LC layer enables pixel colour to be electronically controlled through an applied voltage across the device, where LC re-orientation leads to tunable mixing of the relative contributions from the plasmonic colour input. Furthermore, exploiting the strong surface anchoring effects between an aluminium surface and LC molecules a twisted nematic LC cell, using a metallic grating as a combined colour filter, electrode and alignment layer, was shown to act a variable amplitude colour filter. The colour of these pixels was improved greatly utilising a grating-insulator-grating structure unique to this work. Second, a new process for fabricating aluminium nano-rod structures embedded in an elastomeric medium, with high spatial accuracy, is presented. The process is used to create nano-rod plasmonic resonator arrays whose optical properties may be altered by mechanical deformation. The pattern transfer process is further utilised to create dynamic optical elements, including nano-rod arrays for colour filters, tunable focal length Fresnel zone plates and photon sieves, and stretchable holograms with dynamic replay fields.

The diploma thesis is aimed to excitation and detection of surface plasmon polaritons by visible light. First of all, we will briefly remind some basic principles like waves, electromagnetic wave, light on the interface and optical properties of metals. By using these principles we show presence of surface plasmon polaritons states. After the explanation of their properties there will be clearly visible reasons for aplications of the special excitationand detection methods. We will describe especially the prism coupling, periodic grating coupling and SNOM. Two last sections deal with computer simulations and experiments related to these methods. This means we can exemplify some knowledge presented in previous chapters. Results of simulations are compared with the experiment where we study the excitations of surface plasmon polaritons by periodic grating on aluminium surface.