In this thesis the interaction of ultrashort laser pulses with metal nanostructures is investigated via two different phenomena: coherent acoustic oscillations of nanoparticles and generation of THz pulses on metal surfaces. Both of these effects rely on the collective oscillations of free conduction electrons in metal surfaces, plasmons. The field of plasmonics gained a great interest in the last twenty years due to the unique properties of these surface modes. It is the effects of the resonant response of plasmonic structures to incident electromagnetic wave, in particular, in visible and infrared bands and the concentration of the electromagnetic field in small subwavelength regions with significant enhancement of the incident field that make plasmonics so attractive for various applications, such as biochemical sensing, enhanced fluorescence, surface-enhanced Raman scattering, and second harmonic generation, amongst others. Investigation of the coherent particle vibrations is performed using the pump-probe technique which allows measurement of the transient transmission signals. The expansion and subsequent contraction of the nanoparticle following the ultrashort laser pulse excitation lead to a shift of the plasmon band which can be traced by transient spectroscopy. We have investigated the effect of the particle thickness on the frequency of the fundamental vibrational mode. In addition, we measured the vibrational particle response during the particle shape deformation, both symmetrical and asymmetrical. Exploration of the THz generation phenomena on plasmonic structures was performed using THz time-domain spectroscopy, the method which allows tracing of the generated THz field in the time-domain. We were able for the first time to measure the THz pulses generated from arrays of metal nanoparticles. Our observations verify the role of the particle plasmon mode in the generation of THz pulses. In addition, by exploring the dependence of the THz emission on the femtosecond pulse intensity we showed a high nonlinearity in the THz generation mechanism. The experimental results were assessed in the context of a recently proposed model where the THz radiation is generated via the acceleration of the ejected electrons by ponderomotive forces. To reveal another proposed mechanism of the THz generation from plasmonic structures, namely optical rectification, we investigated the THz generation and electron emission from the arrays of nanoparticles and nanoholes. Our results suggest that both mechanisms may contribute to generation of THz pulses from the same sample under different illumination conditions. In addition to periodic arrays of nanoparticles and nanoholes, THz generation from random metal-dielectric films was investigated. The microstructuring of such films allowed selective THz frequency generation which was explained by a model of dipole THz emitters. In addition, the effects of low temperature and pressure on the THz generation efficiency were investigated.

In this dissertation, an all-fiber-based single frequency nanosecond pulsed laser system at ~ 1918.4 nm in master-oscillator-power-amplifier (MOPA) configuration is present. The nanosecond pulse seed is achieved by directly modulating a continuous wave (CW) single frequency fiber laser using a fast electro-optical modulator (EOM) driven by an arbitrary waveform generator (AWG). One piece of single mode, large core, polarization-maintaining (PM) highly thulium-doped (Tm-doped) germanate glass fiber (LC-TGF) is used to boost the pulse power and pulse energy of these modulated pulses in the final power amplifier. This laser system can work in both high power and high energy regime: in high power regime, to the best of our knowledge, the highest average power 16 W and peak power 78.1 kW are achieved for single frequency transform-limited ~2.0 ns pulses at 500 kHz and 100 kHz repetition rate, respectively: In high energy regime, nearly 1 mJ and half mJ pulse energy is obtained for ~15 ns pulses at 1 kHz repetition rate and 5 kHz repetition rate, respectively. Theoretical modeling of the large-core highly Tm-doped germanate glass double-cladding fiber amplifier (LC-TG-DC-FA) is also present for 2&mum nanosecond pulse amplification. A good agreement between the theoretical and experimental results is achieved. The model can simulate the evolution of pump power, signal energy, pulse shape and the amplified stimulated emission (ASE) in the amplifier. It can also be utilized to investigate the dependence of the stored energy in the LC-TGF on the pump power, seed energy and repetition rate, which can be used to design and optimize the LC-TG-DC-FA to achieve higher pulse energy and average power. Two channel of high energy nanosecond pulses (at 1918.4 nm and 1938 nm) are utilized to generate THz wave in a quasi-phase-matched (QPM) gallium arsenide (GaAs) based on difference frequency generation. THz wave with ~ 5.4μW average power and ~18 mW peak power has been achieved. Besides, one model is built to simulate a singly resonated THz parametric oscillator. The threshold, the dependence of output THz energy on pump energy has been investigated through this model. One pump enhanced THz parametric oscillator has been proposed. The enhancement factor of the nanosecond pulses in a bow-tie ring cavity has been calculated for different pulse duration, cavity length and the transmission of the coupler. And the laser resonances in the ring cavity have been observed by using a piezo to periodically adjust the cavity length. We also build an all-fiber thulium-doped wavelength tunable mode-locked laser operating near 2&mum. Reliable self-starting mode locking over a large tuning range (>50 nm) using fiber taper based carbon nanotube (FTCNT) saturable absorber (SA) is observed. Spectral tuning is achieved by stretching another fiber taper. To the best of our knowledge, this is the first demonstration of an all-fiber wavelength tunable mode-locked laser near 2&mum.

In dieser Arbeit wird die ultraschnelle Dynamik von Leitungsbandelektronen in Halbleitermaterialien mit Hilfe nichtlinearer Terahertz-Spektroskopie erforscht. Insbesondere wird n-dotiertes Galliumarsenid bei mittleren Dotierdichten zwischen 10^(16) cm^(-3) und 10^(17) cm^(-3) untersucht. Für die Erzeugung intensiever THz Strahlung wurde eine neuartige Quelle entwickelt, die THz Transienten mit nur einer Oszillationsperiode und maximalen Feldamplituden von mehr als 400 kV/cm liefert. Diese THz-Quelle benutzt ultrakurze optische Laserpulse aus einem Ti:Saphir Oszillator. Zusätzlich wurde ein neuartiger zwei-Farben Anrege-Abtast Experimentierplatz aufgebaut, der zweidimensionale, zeitaufgelöste Messungen im mittleren und fernen Infrarotbereich ermöglicht. Feldionisation flacher, neutraler Störstellen im Galliumarsenid-Gitter mittels intensiver, ultrakurzer THz Impulse und die anschliessende kohärente, strahlende Rekombination von Elektronen in die Störstellen-Grundzustände bei Raumtemperatur wird gezeigt. Der superradiante Zerfall der nichtlinearen Polarisation führt zur Abstrahlung eines kohärenten Signals mit Lebensdauern von über einer Pikosekunde. Solche nichtlinearen Signale, die 10-fache Lebensdauern im Vergleich zum linearen Fall aufweisen, wurden in dieser Arbeit zum ersten Mal gemessen. Bei niedrigen Temperaturen und THz Feldstärken unter 5 kV/cm werden Rabi-Oszillationen an Übergängen in flachen Störstellen demonstriert. Zum ersten Mal konnte die polare Elektron-LO-Phonon Wechselwirkung im quantenkinetischen Regime direkt gemessen werden. Die quasi-instantane Beschleunigung von Leitungsbandelektronen im polaren Galliumarsenid-Gitter und die anschließende Messung der Transmission im mittleren Infrarot-Bereich, zeigen eine Modulation der Transmission entlang der Anrege-Abtast Verzögerung mit der Frequenz des LO Phonons. Diese Oszillation ist ein direktes Maß der relativen Phase zwischen der Elektronenbewegung und der umgebenden Phonon Wolke. Quantenkinetische Modellrechnungen reproduzieren vollständig die beobachteten Effekte. / In this thesis, the ultrafast dynamics of conduction band electrons in semiconductors are investigated by nonlinear terahertz (THz) spectroscopy. In particular, n-doped gallium arsenide samples with doping concentrations in the range of 10^16cm^(-3) to 10^17 cm^(-3) are studied. A novel source for the generation of intense THz radiation is developed which yields single-cycle THz transients with field amplitudes of more then 400 kV/cm. The THz source uses ultrashort optical laser pulses provided by a Ti:sapphire oscillator. In addition, a two-color THz-pump mid-infrared-probe setup is implemented, which allows for two-dimensional time-resolved experiments in the far-infrared wavelength range. Field ionization of neutral shallow donors in gallium arsenide with intense, ultrashort THz pulses and subsequent coherent radiative recombination of electrons to impurity ground states is observed at room temperature. The superradiant decay of the nonlinear polarization results in the emission of a coherent signal with picosecond lifetimes. Such nonlinear signals, which exhibit a lifetime ten times longer than in the linear regime are observed for the first time. At low temperatures and THz field strengths below 5 kV/cm, Rabi flopping on shallow donor transitions is demonstrated. For the first time, the polar electron-LO phonon interaction is directly measured in the quantum kinetic transport regime. Quasi-instantaneous acceleration of conduction band electrons in the polar gallium arsenide lattice by the electric field of intense THz pulses and subsequent probing of the mid-infrared transmission reveals a modulation of the transmission along the THz-mid-infrared delay coordinate with the frequency of the LO phonon. These modulations directly display the relative phase between the electron motion and its surrounding virtual phonon cloud. Quantum kinetic model calculations fully account for the observed phenomena.