Doctor of Philosophy / Department of Physics / Zenghu Chang / It is still a dream to image the dynamics of electrons in atoms and molecules experimentally. This is due to the fact that such motion takes place in an ultra-short time scale; for example, an electron moves around the Bohr orbit in about 150-as (1 as = 10 -18 s), and pulses much shorter than this limit are not currently available to probe such fast dynamics. In recent years, an isolated single attosecond pulse has been produced by extracting the cutoff of harmonic spectrum driven by a laser pulse as short as ~ 5fs (1fs =10-15 s). But, these pulses are still too long in order to make the dream come true. Here, we study the possibility of generation of a much shorter and wavelength tunable single attosecond pulse by using polarization gating. In the experiment, we compressed ~30fs pulses from the laser amplifier down to ~6fs and characterized them. These linearly polarized pulses were converted to ellipticity varying pulses, and by exploiting the property of the strong dependence of the harmonic signal with the ellipticity of the laser, an XUV supercontinuum was produced in the harmonic spectrum which could support 60-as pulses. The bandwidth of such a supercontinuum, and therefore the duration of the attosecond pulses, is limited mainly by the currently available energy of the driving laser pulses at few cycle limits. In this project, we present an approach which allowed us to scale up the energy of such pulses by a factor of 1.5 in “Hollow Core Fiber / Chirped Mirrors Compressor”. Finally, in order to temporarily characterize the attosecond pulses we designed and built an “Attosecond Streak Camera”. Most of such cameras to date are limited to measuring a 1 dimensional energy spectrum and have only a few degrees of acceptance angle. Our camera is capable of measuring 2d momentum of the photoelectrons with large acceptance angle, for example ~ 65o at the photoelectron of energy ~15 eV. Recently, we observed the sidebands in addition to the main peaks in their laser assisted XUV photoelectron spectrum. The single attosecond pulses, after being characterized with this high speed camera, can be used to explore the dynamics of electrons at the attosecond scale.

This Thesis is devoted to theoretical investigation of the effective magnetic properties of nonlinear metamaterials, based on resonant conductive elements.A general expression for the effective bulk ermeability in the microwave frequency range is derived. Frequency dispersion of the permeability is studied and recommendations for optimisation of metamaterials with negative permeability are given. The results are supported with numerical simulation of the finite metamaterial sample.Next, a metamaterial possessing nonlinear magnetic responseowing to nonlinear electronic components, inserted into resonant conductive elements, is proposed. For the limit of low nonlinearity, the arising quadratic nonlinear susceptibility is calculated; it is shown how it is controlled by the properties and arrangement of the structure elements as well as by the type and characteristics of the insertion.For the insertions operating in essentially nonlinear regime, when a nonlinear magnetic susceptibility cannot be introduced, an approach is developed for analyzing three-wave coupling processes with a strong pump wave and two weak signals. Peculiarities of coupling, arising from use the insertions with variable resistance or variable capacitance are discussed. Estimates are given that extremely strong nonlinear coupling can be achieved using typical diodes reported in literature.Finally, it is demonstrated how the metamaterial band gap can be tuned, and the resulting metamaterial switching between transmitting, reflecting and absorbing states is described. The details appear to depend drastically on the type of nonlinear components inserted into the resonant conductive elements. Relying on practical estimates, it is predicted that the transmittance of a metamaterial slab can be modulated by several orders of magnitude already using a slab with thickness equal to one microwave wavelength in vacuum.

We develop a theory of vectorial wave coupling in cubic photorefractive crystals placed in an alternating ac-field to enhance the nonlinear response. First we analytically and numerically investigate the dependences of the first Fourier harmonics of the space-charge field, induced in an AC-biased sillenite crystal by a light-interference pattern, on the light contrast m. The data obtained was used to extend the vectorial beam-coupling theory on the whole contrast region. In particular, we proved in the general case that despite of essential differences between thediffusion and AC nonlocal responses the later keeps the light interference fringes straight during the interaction. This fundamental feature allows, under certain restrictions, to reduce the nonlinear problem of vectorial coupling to the known linear problem of vectorial Bragg diffraction from a spatially uniform grating, which admits an exact solution. As a result, the nonlinear vectorial problem can be effectively solved for a number of practically important cases.The developed theory was applied to describe the transformation of a momentary phase changes of one of the input beams into the output intensity modulation (so-called grating translation technique). In contrast to the previous studies, we take into account the change of the space-charge field amplitude across the crystal (the coupling effects). The theory developed is employed to optimize the conditions for the linear signal detection under polarization filtering for the transverse and longitudinal optical configurations. We also analyze the possibility of the linear detection without polarization filtering.Illumination of AC-biased photorefractive BTO crystals with a coherent light beam results in development of strong nonlinear scattering. We investigate the angular and polarization characteristics of the scattered light for the diagonal optical configuration and different polarization states of the pump.

The present work broaches the physics of light-matter interaction, chiefly using nonlinear optical spectroscopy in a newly developed framework termed as Photon Management Concept. This way, existing fragments dealing with specific properties of harmonic and upconversion nanoparticles (HNPs/UCNPs) are consolidated into a full and coherent picture with the primary goal of understanding the underlying physical processes and their impact on the application side, especially in terms of imaging techniques, via suitable experimental and numerical studies. Contemporary optical setups involving contrast-enhancing agents are frequently limited in their excitation and detection configurations owing to a specialization to a select number of markers. As a result, the bandwidth of experimental methods and specimens that may be investigated is severely restricted in a large number of state-of-the-art setups. Here, an alternative approach involving HNPs and UCNPs, respectively, is presented providing an overview from their synthesis to optical characterization and to potential fields of application. Based on their inherent flexibility based on their nonlinear optical response, especially in terms of wavelength and intensity tunability, the PMC alleviates prevalent limitations by dynamically adapting the setup to a sample instead of the preliminary culling to a reduced number of eligible specimens that must not change their optical properties significantly during investigation. The use of HNPs supersedes such concerns due to their nearly instantaneously generated, strongly anti-Stokes shifted, coherent emission capable of producing radiation throughout the visible spectral range, including infrared and ultraviolet wavelengths. This way, HNPs transcend the traditional field of imaging and introduces potential applications in optomanipulation or holographic techniques. Thorough (nonlinear) optical characterization of UCNPs and alkali niobate HNP ensembles is performed to assess the fundamental physical mechanisms interwoven with numerical studies leading to their wide-ranging applicability. Final remarks show that HNPs are ideal candidates for realization of the PMC and yet hold an even further potential beyond current prospects.

In der vorliegenden Arbeit werden die nichtlinearen optischen Eigenschaften der Materialien Lithiumniobat und Di-Zinn-Hexathiohypodiphosphat aufgrund der Suszeptibilität 3. Ordnung und kleiner Polaronen untersucht. Zudem wird gezeigt, dass die Interferenz verschiedenfarbiger Laserpulse die Aufzeichnung von statischen und dynamischen holographischen Gittern ermöglicht. Ein Teil dieser Arbeit ist in den im Anhang angegebenen 6 Publikationen bereits veröffentlicht. Lithiumniobat wird mit einer Erweiterung des Z-Scan Experiments untersucht, welches die Pulslängenabhängige Messung der nichtlinearen Absorption und der nichtlinearen Brechungsindexänderung ermöglicht. Dabei konnte festgestellt werden, dass bei sehr kurzen Pulslängen von 70 fs ein Effekt der Polaronen auf die nichtlineare Absorption vernachlässigbar ist und die Zwei-Photonen-Absorption die nichtlineare Absorption dominiert. Mit größerer Pulslänge gibt es allerdings Abweichungen zwischen der Theorie der Zwei-Photonen-Absorption und den Messergebnissen. Mit der Entwicklung eines Polaronen-Anregungs-Modells, welches eine polaronische Absorption aufgrund wiederholtem optisch induziertem Hopping annimmt, konnte dieser Effekt konsistent erklärt werden. Die Messungen der nichtlinearen Brechungsindexänderung lassen darauf schließen, dass sowohl freie Ladungsträger als auch kleine Polaronen neben der Suszeptibilität 3. Ordnung einen Einfluss auf die Brechungsindexänderung haben, da eine nichtlineare Abhängigkeit von der Intensität auch bei Pulslängen von 70 fs festgestellt werden konnte. Analog dazu konnte in Di-Zinn-Hexathiohypodiphosphat ein großer Zwei-Photonen-Absorptionskoeffizient festgestellt werden, welcher für Photonenenergien nahe der Bandkante Werte zeigt, die größer sind als theoretischen Überlegungen zeigen. Eine transiente Absorption nach optischer Anregung, gemessen durch ein Anreg-Abtast-Experiment, sowie Literatur legen nahe, dass in Di-Zinn-Hexathiohypodiphosphat gebundene Lochpolaronen durch optische Anregung entstehen können. Durch den hohen Zwei-Photonen-Absorptionskoeffizienten konnte das Aufzeichnen eines kontrastreichen, dynamischen Amplitudengitters mittels Femtosekundenpulsen gezeigt und nachgewiesen werden. Die Kürze der Femtosekundenpulse ermöglicht aber nicht nur das Aufzeichnen eines Zwei-Photonen-Absorptionsgitters aufgrund der hohen Intensitäten, sondern erlaubt zudem die Beobachtung von Interferenz zwischen verschiedenfarbigen Pulsen. In der Zeitspanne der Pulslänge beträgt die Bewegung der Interferenzstreifen, welche in der Größenordnung der Lichtgeschwindigkeit liegt, nur ein Bruchteil der Streifendistanz, sodass das Interferenzmuster eingefroren und beobachtbar erscheint. Somit lassen sich statische Hologramme in holographischen Filmen, wie auch dynamische Hologramme aufzeichnen. Über ein dynamisches holographisches Gitter mittels Zwei-Photonen-Absorption konnte so eine Frequenzkonversion durch Dopplerverschiebung in Lithiumniobat gezeigt werden.