Waveguide architectures were inscribed within two different stimuli-responsive hydrogels capable of actuation. An electroactive hydrogel, which deforms when placed within an electric field, is demonstrated as a method for remote actuation and steering of light outputs. Lattices of waveguide with diameters on the microscale were embedded within hydrogel prisms, achieved through a nonlinear light propagation process known as self-trapping. This process is a result of balance between the natural divergence of light and self-focusing effects caused by an irreversible positive refractive index change during photopolymerization. Waveguiding structures are inscribed in the material because of this process. Square (2D) and near-cubic (3D) lattices were inscribed in hydrogel prisms, demonstrating the ability to remotely steer one or two light outputs simultaneously using an electric field. The overall optical effect is reminiscent of camouflaging techniques observed in marine creatures (ie. cephalopods). Additionally, a novel volumetric 3D printing technique previously demonstrated by the Saravanamuttu group was implemented to fabricate hydrogel cylinders capable of photothermal actuation. Coupling a thermoresponsive hydrogel material with a photoabsorber, areas irradiated by a light source are observed to contract. These contractions lead to the deflection of waveguiding cylinders towards the light source, reminiscent of the phototropic behaviours observed in particular plants (ie. sunflowers). The results of these studies provide insight for the fabrication of functional materials through nonlinear light propagation. Understanding these systems could provide knowledge for the fabrication of other stimuli-responsive materials with light-guiding properties. / Thesis / Master of Science (MSc)

Polymer matrices doped with a dispersion of noble metal nanoparticles combine the strong plasmon resonance-based optical signatures of the latter with the flexibility and processability of the former. We have developed a nonlinear lithographic technique to generate large populations of epoxide waveguides containing a uniform dispersion of Au nanoparticles. The method is based on the self-trapping of multiple beams of white light propagating through a catonic polymerizable matrix doped with a gold salt, initiating the polymerization of epoxide moieties and simultaneously the in situ synthesis of elemental Au nanoparticles. Each white light filament inscribes a cylindrical waveguide, leading to an array of metallodielectric waveguides. Field of view (FOV) measurements indicate that the metallodielectric waveguide array has a nearly 59 % increase in FOV relative to its all-dielectric counterparts and can be tuned through the concentration of Au nanoparticles and the optical intensities employed to generate waveguides. / Thesis / Master of Science (MSc)

The nonlinear propagation of a visible, continuous wave laser beam was studied in three types of polymer systems that harness photochemical reactions: (i) a photopolymerization to create permanent self-written structures, (ii) a photo-oxidation hosted within a polymer matrix and (iii) a reversible photoisomerization that triggers the contraction of a photoresponsive hydrogel. The process of self-trapping was characterized by monitoring the spatial intensity profiles over time. The mechanism of each material was determined with a series of control experiments in order to confirm the nature of the nonlinear response, including their reversibility and intensity-dependence. These observations led to the study of interactions between self-trapped beams. Two beams under linear conditions will pass through one another, but two beams travelling in a nonlinear medium will interact and influence one another. The interactions of two beams introduced into the aforementioned photochemical systems were investigated and revealed a rich diversity of phenomena including: (i) the attraction between beams, (ii) merging of beams into a single waveguide, (iii) nonlocal attraction between beams, (iv) orbiting of beams, (v) switching of beam positions, and (vi) inhibition of the self-trapping of a neighbouring beam. Each observation is dependent on a detailed understanding of the underlying mechanism of refractive index change. Numerical simulations supplement some of these experiments and provide further evidence for the nonlinear mechanisms. The formation of permanent self-written structures with these nonlinear waves offers the opportunity to create seamless 3D printed materials with prismatic geometries. Several macroscopic objects were constructed using nonlinear waves from incoherent LEDs and amplitude masks. Decomposition of 3D objects into prismatic elements was carried out using an algorithm that breaks an object into individual pieces. Using a multi-step printing process, several prismatic elements can be combined to form a target object. The results of these experimental and theoretical studies improve upon the current understanding of the dynamics of nonlinear light propagation in photochemical systems. These insights may allow us to harness other nonlinear effects and develop new materials for applications such as optical communication, computing and 3D printing. / Thesis / Doctor of Science (PhD) / The nonlinear propagation of a visible, continuous wave laser beam was studied in three types of polymer systems that harness photochemical reactions: (i) a photopolymerization to create permanent self-written structures, (ii) a photo-oxidation hosted within a polymer matrix and (iii) a reversible photoisomerization that triggers the contraction of a photoresponsive hydrogel. Photochemical changes to the material lead to self-induced light-guiding structures that influence the behaviour of light. These self-trapped beams can interact with one another inside of a nonlinear medium, giving rise to a rich diversity of phenomena including: (i) the attraction between beams, (ii) merging of beams into a single waveguide, (iii) nonlocal attraction between beams, (iv) orbiting of beams, (v) switching of beam positions, and (vi) inhibition of the self-trapping of a neighbouring beam. Each observation is dependent on a detailed understanding of the underlying mechanism of refractive index change. Numerical simulations supplement some of these experiments and provide further evidence for the nonlinear mechanisms. The formation of permanent self-written structures with these nonlinear waves offers the opportunity to create seamless 3D printed materials with prismatic geometries. Several macroscopic objects were constructed using nonlinear waves from incoherent LEDs and amplitude masks. Decomposition of 3D objects into prismatic elements was carried out using an algorithm that breaks an object into individual pieces. Using a multi-step printing process, several prismatic elements can be combined to form a target object. The results of these experimental and theoretical studies improve upon the current understanding of the dynamics of nonlinear light propagation in photochemical systems. These insights may allow us to harness other nonlinear effects and develop new materials for applications such as optical communication, computing and 3D printing.

There is a strong push worldwide to develop multi-Joule femtosecond duration laser pulses at wavelengths around 3.5-4 and 9-11 mu m within important atmospheric transmission windows. We have shown that pulses with a 4 mu m central wavelength are capable of delivering multi-TW powers at km range. This is in stark contrast to pulses at near-IR wavelengths which break up into hundreds of filaments with each carrying around 5 GW of power per filament over meter distances. We will show that nonlinear envelope propagators fail to capture the true physics. Instead a new optical carrier shock singularity emerges that can act to limit peak intensities below the ionization threshold leading to low loss long range propagation. At LWIR wavelengths many-body correlations of weakly-ionized electrons further suppress the Kerr focusing nonlinearity around 10 mu m and enable whole beam self-trapping without filaments.

The dissociation of hydrogen molecules at surfaces is the first step in the absorption process. If the absorbing material is covered by an oxide, this layer will determine the effective uptake rate of an underlying absorbing material. This effect is illustrated when determining the rate of transport of hydrogen through amorphous aluminium oxide layers. The transport rate was determined to be strongly thickness dependent. Hydrogen absorbed in a transition metal causes a volume expansion generated by a strain field around the absorbed hydrogen. This strain field causes a self-trapping of the hydrogen and a temperature dependent distribution in the atomic distances. The local strain field generated by the self-trapping process is found to be crucial for understanding both the hydrogen induced volume expansion as well as the diffusion of hydrogen. Ab-initio molecular dynamics simulations were used to reveal the temperature dependence of the unbinding of the hydrogen and the local strain field and its influence on the diffusion rate. The symmetry of the local strain field is also important for phase formation in metallic films and superlattices which are clamped to a substrate. As the thicknesses reduced from 50 to 10 nm thick vanadium films, substantial finite size effects become apparent in the phase diagrams. The volume change associated with the strain field cannot be accurately measured using x-ray diffraction because of its sensitivity to local arrangements of atoms. X-ray and neutron reflectivity were found to be more reliable probes of global effects of the sumof the local strainfields. Finite size effects in extremely thin V layers were also explored in metallic superlattices composed of iron and vanadium. The co-existence region, composed of a hydrogen gas and a solid-like phase, was found to be suppressed by at least 100 K to below 300 K. The hydrogen-hydrogen interaction can also be influenced by the electronic states in the non hydrogen absorbing layers, as demonstrated when comparing hydrogen absorption in Fe/V and Cr/V superlattices. / Felaktigt tryckt som Digital Comprehensive Summaries of Uppsala Dissertations from the Faculty of Science and Technology 728

The experimental studies presented in this thesis deal with the photoluminescence intermittency of semiconductor quantum dots in different dielectric environments. Detailed analysis of intermittency statistics from single capped CdSe/ZnS, uncapped CdSe and water dispersed CdSe/ZnS QDs in different matrices provide experimental evidence for the model of photoionization with a charge ejected into the surrounding matrix as the source of PL intermittency phenomenon. The distribution of the dark state lifetimes can be described by a power law over a wide range while that of bright state can be described by a power law at shorter times followed by an exponential decay. The lifetimes of the bright and dark states are influenced by the dielectric properties of the surrounding environment. Our experimental results show that the lifetime of the dark state increases with the dielectric constant of the matrix. This is very clear from the linear correlation between αoff and f (ε). We propose a self-trapping model to explain the increase of dark state lifetimes with the dielectric constant of the matrix. A charge will be more stabilized in a medium with high dielectric constant. An energetically more favourable state for an electron in a high dielectric medium decreases the return probability which eventually increases the duration of the off-time. Moreover, the self-trapping model establishes a general model for distribution of states in a matrix. We like to mention, that in the case of bright states, a qualitative observation is the cross over of the on-time power law behavior to an exponential one. The power law part of the decay is nearly matrix independent while the exponential decay, which limits the maximum on-time, strongly depends on dielectric properties of the environment. The exponential part of the on-time probability decays much faster in a high dielectric medium and there exists a linear relation between the time constant of the exponential decay and f (ε). Theoretical background has been provided for the observed results using the recently published DCET model which correlates PL intermittency of QDs with properties of the environment. This supports our previous conjecture of a general model for matrix controlled blinking process. The disagreement between experimentally observed dependence of αoff and f (ε) for different matrices with that of the static tunnelling model proposed by Verberk is due to the fact that the tunneling model considers only an electron transfer between a QD and spatially distributed trap states in vacuum. These states are already stabilized states. It does not assume any medium in between. Therefore, matrix dependent blinking kinetics can not be explained quantitatively by tunneling model even though tunneling between a QD and spatially distributed trap states gives a power law distribution for the blinking kinetics. DCET is a more general (dynamic) model. The bright and dark state parabolas contain QD, charge and the matrix. Therefore, this model could in principle explain matrix dependent blinking kinetics in a better way, for example, the energy difference between the minima of the bright and dark state parabolas (-ΔG0) is defined by the stabilization energy of the system provided by the matrix. However, due to lack of the relevant intrinsic parameters we did not compare this relationship and dependence qualitatively. / Betrachtet man die Fluoreszenz einzelner Farbstoffmoleküle oder Halbleiternanokristalle bei kontinuierlicher Anregung, so stellt man fest, dass die im Zeitverlauf beobachtete Intensität einer stochastischen Variation unterliegt, d. h. dass das Chromophor zwischen emittierenden und nicht emittierenden Zuständen, auch Hell- und Dunkelzuständen genannt, hin- und herschaltet. Dieses als Blinken bekannte Phänomen ist physikalisch wie auch technologisch herausfordernd, lässt es doch einerseits die Realisierbarkeit einer Reihe von quantenoptischen Anwendungen, so z. B. auf dem Gebiet der Quantenkryptographie, dem Quantum Computing oder der optischen Schaltungstechnik auf Basis einzelner Quantenobjekte, in naher Zukunft möglich erscheinen. Andererseits setzt es gewissen Anwendungen, die auf die permanente Sichtbarkeit des Chromophors aufbauen, Grenzen, so zum Beispiel der Verwendung als Lumineszenzmarker in der medizinischen Diagnostik. Weiterhin ist festzustellen, dass das Blinken kritisch von den äußeren Bedingungen und von den Umgebungsparametern abhängt. Aus diesen und anderen Gründen ist ein fundamentales Verständnis der physikalischen Ursachen und der Wechselwirkungsprozesse unerlässlich. Die Forschung dazu steckt noch in den Kinderschuhen. Basierend auf umfangreiche Messungen der Fluoreszenzzeitreihen einzelner Nanokristalle aus CdSe und CdSe/ZnS in verschiedenen Umgebungen, zeigt diese Dissertation exemplarisch den Einfluss der Dielektrizitätsparameter auf das Blinken. Zur Erklärung des Sachverhalts wird ein so genanntes Self-Trapping-Modell zu Rate gezogen. Demnach kommt es zu einer Ionisation des Quantenobjekts und anschließender Ladungstrennung, woraufhin die abgetrennte Ladung für eine gewisse Zeit in der Umgebung lokalisiert bleibt. Die Dauer der Lokalisierung und damit der emittierenden und nicht emittierenden Perioden hängt von der dielektrischen Funktion des umgebenden Materials ab. Dies ist als direkter Nachweis für den photoinduzierten Ladungstransfer als Ursache des Fluoreszenzblinkens zu deuten. Die Arbeit demonstriert, dass die experimentellen Zeitreihen die charakteristischen Merkmale eines diffusionsgesteuerten Ladungstransferprozesses besitzen und nimmt dabei den gegenwärtigen wissenschaftlichen Diskurs über geeignete theoretische Modelle des Fluoreszenzblinkens auf.

My dissertation treats the physics of ultracold gases, in particular of Bose-Einstein condensates with long-ranged interactions induced by admixing a small fraction of a Rydberg state to the atomic ground state. The resulting interaction leads to the emergence of supersolid states and to the self-trapping of a Bose-Einstein condensate.

The experimental studies presented in this thesis deal with the photoluminescence intermittency of semiconductor quantum dots in different dielectric environments. Detailed analysis of intermittency statistics from single capped CdSe/ZnS, uncapped CdSe and water dispersed CdSe/ZnS QDs in different matrices provide experimental evidence for the model of photoionization with a charge ejected into the surrounding matrix as the source of PL intermittency phenomenon. The distribution of the dark state lifetimes can be described by a power law over a wide range while that of bright state can be described by a power law at shorter times followed by an exponential decay. The lifetimes of the bright and dark states are influenced by the dielectric properties of the surrounding environment. Our experimental results show that the lifetime of the dark state increases with the dielectric constant of the matrix. This is very clear from the linear correlation between αoff and f (ε). We propose a self-trapping model to explain the increase of dark state lifetimes with the dielectric constant of the matrix. A charge will be more stabilized in a medium with high dielectric constant. An energetically more favourable state for an electron in a high dielectric medium decreases the return probability which eventually increases the duration of the off-time. Moreover, the self-trapping model establishes a general model for distribution of states in a matrix. We like to mention, that in the case of bright states, a qualitative observation is the cross over of the on-time power law behavior to an exponential one. The power law part of the decay is nearly matrix independent while the exponential decay, which limits the maximum on-time, strongly depends on dielectric properties of the environment. The exponential part of the on-time probability decays much faster in a high dielectric medium and there exists a linear relation between the time constant of the exponential decay and f (ε). Theoretical background has been provided for the observed results using the recently published DCET model which correlates PL intermittency of QDs with properties of the environment. This supports our previous conjecture of a general model for matrix controlled blinking process. The disagreement between experimentally observed dependence of αoff and f (ε) for different matrices with that of the static tunnelling model proposed by Verberk is due to the fact that the tunneling model considers only an electron transfer between a QD and spatially distributed trap states in vacuum. These states are already stabilized states. It does not assume any medium in between. Therefore, matrix dependent blinking kinetics can not be explained quantitatively by tunneling model even though tunneling between a QD and spatially distributed trap states gives a power law distribution for the blinking kinetics. DCET is a more general (dynamic) model. The bright and dark state parabolas contain QD, charge and the matrix. Therefore, this model could in principle explain matrix dependent blinking kinetics in a better way, for example, the energy difference between the minima of the bright and dark state parabolas (-ΔG0) is defined by the stabilization energy of the system provided by the matrix. However, due to lack of the relevant intrinsic parameters we did not compare this relationship and dependence qualitatively. / Betrachtet man die Fluoreszenz einzelner Farbstoffmoleküle oder Halbleiternanokristalle bei kontinuierlicher Anregung, so stellt man fest, dass die im Zeitverlauf beobachtete Intensität einer stochastischen Variation unterliegt, d. h. dass das Chromophor zwischen emittierenden und nicht emittierenden Zuständen, auch Hell- und Dunkelzuständen genannt, hin- und herschaltet. Dieses als Blinken bekannte Phänomen ist physikalisch wie auch technologisch herausfordernd, lässt es doch einerseits die Realisierbarkeit einer Reihe von quantenoptischen Anwendungen, so z. B. auf dem Gebiet der Quantenkryptographie, dem Quantum Computing oder der optischen Schaltungstechnik auf Basis einzelner Quantenobjekte, in naher Zukunft möglich erscheinen. Andererseits setzt es gewissen Anwendungen, die auf die permanente Sichtbarkeit des Chromophors aufbauen, Grenzen, so zum Beispiel der Verwendung als Lumineszenzmarker in der medizinischen Diagnostik. Weiterhin ist festzustellen, dass das Blinken kritisch von den äußeren Bedingungen und von den Umgebungsparametern abhängt. Aus diesen und anderen Gründen ist ein fundamentales Verständnis der physikalischen Ursachen und der Wechselwirkungsprozesse unerlässlich. Die Forschung dazu steckt noch in den Kinderschuhen. Basierend auf umfangreiche Messungen der Fluoreszenzzeitreihen einzelner Nanokristalle aus CdSe und CdSe/ZnS in verschiedenen Umgebungen, zeigt diese Dissertation exemplarisch den Einfluss der Dielektrizitätsparameter auf das Blinken. Zur Erklärung des Sachverhalts wird ein so genanntes Self-Trapping-Modell zu Rate gezogen. Demnach kommt es zu einer Ionisation des Quantenobjekts und anschließender Ladungstrennung, woraufhin die abgetrennte Ladung für eine gewisse Zeit in der Umgebung lokalisiert bleibt. Die Dauer der Lokalisierung und damit der emittierenden und nicht emittierenden Perioden hängt von der dielektrischen Funktion des umgebenden Materials ab. Dies ist als direkter Nachweis für den photoinduzierten Ladungstransfer als Ursache des Fluoreszenzblinkens zu deuten. Die Arbeit demonstriert, dass die experimentellen Zeitreihen die charakteristischen Merkmale eines diffusionsgesteuerten Ladungstransferprozesses besitzen und nimmt dabei den gegenwärtigen wissenschaftlichen Diskurs über geeignete theoretische Modelle des Fluoreszenzblinkens auf.

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L'étude menée dans cette thèse concerne la dynamique de systèmes quantiques hors de l'équilibre, et plus particulièrement leurs propriétés d'intrication. En effet, l'intrication est devenue un concept fondamental dans la physique moderne, grâce notamment au développement de l'information quantique. Nous avons dans un premier temps étudié la dynamique d'un modèle de bosons sur réseau après la trempe de leur potentiel de confinement. Dans la limite de coeur dur, nous avons développé une théorie hydrodynamique qui reproduit parfaitement les différents comportements observés. Nous nous sommes ensuite intéressés à la dynamique de deux spins défauts couplés à une chaîne d'Ising. Dans un premier temps, ces défauts ont été préparés dans un état séparable. Nous avons dans ce cas établi une formule donnant l'évolution temporelle de la matrice de densité réduite, qui nous a permis d'avoir accès à l'intrication créée par l'intermédiaire du couplage à la chaîne. Puis, nous avons considéré le cas de deux spins défauts initialement intriqués, et nous avons étudié l'influence d'un environnement hors de l'équilibre sur leurs propriétés de désintrication. Finalement, la dernière partie de cette thèse est consacrée à l'étude d'un système couplé à un environnement décrit par le processus d'interactions répétées. Nous avons étudié la relaxation du système dans deux régimes temporels différents. Pour des temps courts, l'état est bien décrit par un état stationnaire hors équilibre, dans lequel nous avons mis en évidence les propriétés d’échelle de certaines observables. Enfin, pour des temps longs, le système atteint un état stationnaire d'équilibre composé d'un produit d'états de Bell / The study carried in this thesis concerns the dynamics of out-Of-Equilibrium quantum systems, and more particularly their entanglement properties. Indeed, entanglement became a fundamental concept in modern physics, especially with the development of quantum information. We have in a first part studied the dynamics of a model of bosons on a lattice after the quench of their trapping potential. In the hard-Core limit, we developed an hydrodynamical theory which perfectly reproduced the observed behavior. Then, we have looked at the dynamics of two defect spins coupled to an Ising chain. When these defects have been prepared into a separable state, we have established a formula giving the evolution of the reduced density matrix, allowing us to have access to the entanglement create through the coupling to the chain. We considered then the case of two initially entangled defect spins, and we studied the influence of a non-Equilibrium environment on the disentanglement properties. Finally, the last part of this thesis is devoted to the study of a system coupled to an environment by means of the repeated interactions process. We studied the relaxation of the system in two different time regimes. For short times, the state is well described by a non-Equilibrium-Steady-State, in which we highlighted the scaling properties of some observables. For long times, the system reaches an equilibrium steady state made of a product of Bell states