In this thesis, we studied chirp response and slow light properties in strained saturable Bragg reflector (SSBR). In the part of chirp response studying, we simulated the chirp response of SSBR of pulses with different chirps, and verified the results of related work. The trend of simulation was consistent with experimental result. Therefore firmly believing the broadening or compression ability of chirped incident pulse in SSBR, the pulse compression ability facilitates the mode-locking in laser cavity and generates more narrow pulse. In the studying of slow light properties in SSBR, a home-made pulse shaper system and a cross-correlator system were demonstrated. We control the chirp of the pulse by pulse shaper, and then pulse enter SSBR and reflect from SSBR, and measure the signal distribution in time domain by cross-correlator, finally we can analyze the properties of slow light of SSBR. We have demonstrated the slow light phenomenon was observed as central wavelength of incident pulse approach to resonance absorption of SSBR. In the aspect of chirp control, contrast with negative chirped incident pulse, slower group velocity with larger group delay for positive chirped incident pulse was observed. This could be attributing to absorption increasing which result from more efficient for creating carrier and less-sensitive to the carrier-scattering effect. In addition, we further study power dependence of slow light properties in SSBR under various incident chirps. Increasing group delay with power of incident pulse was performed. In addition, more group delay under saturation was also characterized and analyzed.

In this thesis, a novel method for multi-pulse with equal chirp characteristics and more efficient THz generation through two photon absorption (TPA) are investigated and demonstrated. These are all the first time, for our best knowledge, odd multi-pulses generation and innovative approach for efficient THz through TPA are proposed and studied. By modulating the amplitude and phase of the spatial light modulator with the pulse shaper, the number of multi-pulses can be adjustable without the limitation of even number only. Meanwhile, the chirp properties of the generated pulses are with the same characteristics and tunable also. For the case with bandwidth of 10nm, the generated multi-pulses with equal chirps varying from -20000fs^2 to 20000fs^2 are demonstrated and the results have a good agreement with the theoretical estimation. We also discuss the number of the multi-pulses and inequalities of the amplitude of the pulses are limited by the spectral resolution of SLM within the pulse shaper. Regarding to efficient THz radiation, it can be generated more efficiently from a low-temperature-grown GaAs (LT-GaAs) photoconductive (PC) antenna by taking into account the TPA induced photo-carrier in the photoconductor. A rate-equation-based approach using the Drude-Lorentz model taking into account the band-diagram of LT-GaAs is used for the theoretical analysis. The super-linear power dependent photocurrent clarifies the role of TPA. Previously unnoticed THz pulse features and anomalously increasing THz radiation power rather than saturation were observed. These are in good agreement with the theoretical predictions.

This thesis utilize pulse shaping in characterization of ultra-broad bandwidth laser pulse and multi-pulse generation. Using angle-dithering technique, time-integrating phase-matching bandwidth can be increased significantly even with a thin crystal. We also characterize the pulse by angle-dithered MIIPS( intrapulse interference phase scan ) technique. An addition advantage of using a thick crystal is increased signal strength. In addition, we provide a method to generate multi-pulses and proceed Michelson interferometeric autocorrelator by controlling the spectral amplitude and phase of the pulse. To compare with the past method, the efficiency was obtained from 33% to 80% , and the stability and time resolution of delay time can be improved. We expect this method applied to narrow-band frequency-tunable THz wave genetration will be better.

En vue de la capture de réearrangements électroniques au sein d’une molécule ou au cours de réactions chimiques il est indispensable de développer un dispositif dont la résolution temporelle est attoseconde (as 1 as = 10−18 s). La voie naturelle est de rechercher des impulsions lumineuses dans cette gamme de durée. Leur fréquence centrale doit alors être dans la gamme UVX et couvrir plusieurs dizaines d’eVs. De plus, ses composantes fréquencielles doivent être synchronisées. Le processus de génération d’harmoniques d’ordre élevé (GHE) dans les gaz remplit ces exigences. Pendant ce processus, une impulsion laser de haute intensité est focalisée dans un jet de gaz, où son champ électrique courbe la barrière de potentiel d’un atome et permet l’ionisation tunnel d’un paquet d’ondes électronique (POE). Entrainé par le champ électrique du laser, le POE accélére et acquiert une énergie cinétique élevée. Dans le cas où il repasse au voisinage du coeur ionique cette énergie cinétique peut être émise sous la forme d’un photon UVX. Ces POE explorent la structure et la dynamique de l’ion dans un schéma d’auto-sonde: le POE émis à un instant donné revient lui même ultérieurement sonder l’ion. Plus précisément ce processus d’autosonde donne accès à la valeur complexe du dipôle de recombinaison moléculaire (DRM), lui-même determiné par les structures nucléaire et électronique de l’ion. Le dipôle de recombinaison, en rayonnant des harmoniques, encode ces caractéristiques dans l’amplitude, la phase et l’état de polarisation de l’émission harmonique. Grâce à la nature cohérente de la GHE nous pouvons mesurer ces trois paramètres.L’objectif de ma thèse de doctorat était double. En mettant en oeuvre des techniques avancées de caractérisation de l’amplitude, de la phase et de la polarisation des harmoniques nous avons dans un premier temps étudié la structure électronique de N2 et l’ionisation tunnel multi-canaux induite par le laser. Nous avons montré les reconstructions des plusieurs orbitals moléculaires et révélé la vibration nucléaire ultra-rapide en fonction des canaux d’ionisations. Dans un deuxième temps nous avons étudié la réflectivité et la dispersion de miroirs UVX à compensation de dérive de fréquence, fabriqués sur mesure. Ces miroirs autorisent la mise en forme temporelle d’une impulsion attoseconde, compriment la durée de l’impulsions où introduisent un TOD. Nous avons aussi proposé un nouveau façonneur d’impulsions. / To capture electronic rearrangements inside a molecule or during chemical reactions, attosecond (as, 1 as =10−18 s) time resolution is needed. To create a light pulse with this duration, the central frequency has to be in the XUV range and cover several tens of eVs. Moreover, the frequency components have to be synchronized. The so called High Harmonic Generation (HHG) in gases well suits this task. During this process a high intensity laser pulse is focused in a gas jet, where its electric field bends the potential barrier of an atom allowing an electron wave packet (EWP) to tunnel ionize. Following the electric field of the laser the EWP gets accelerated, gaining a large kinetic energy that may be released as a high energy (XUV) photon in the event of a re-collision with the ionic core. These recolliding EWP probe the structure and dynamics of the core in a self-probing scheme: the EWP, that is emitted by the molecule at a certain time, probes itself later. More precisely, this ”self-probing” scheme gives access to the complex valued recombination dipole moment (RDM) of the molecule which is determined by both the nuclear and electronic structure. The recombination encodes these characteristics into the spectral amplitude, phase and polarization state of the harmonic radiation emitted by the dipole. Due to the coherent nature of HHG it is possible to measure all these three parameters. Moreover, it is in principle possible through a tomographic procedure to reconstruct the radiating orbital.The objective of my thesis was two-fold. By implementing advanced characterization techniques of the harmonic amplitude, phase and polarization we studied i) the electronic structure of N2 and laser induced multi-channel tunnel ionization. We presented the reconstruction of molecular orbitals and revealed the ionization channel dependent ultrafast nuclear vibration. We also studied ii) the reflectivity and dispersion of recently designed chirped XUV mirrors that can shape the temporal profile of attosecond pulses. With these mirrors we could control the spectral phase over 20 eV and compensate the GDD of the harmonics or introduce a TOD. We also proposed a novel attosecond pulse shaper.

This thesis utilized pulse shaping and Gerberg-Saxton algorithm to develop high power tunable narrowband terahertz radiation and applications. By the way of using Freezing algorithm and Gerberg-Saxton, pulse width, pulse duration, pulse position and pulse number can be controlled. The pulse train can be pumping source of high power tunable narrowband terahertz radiation, by avoid the saturations and different pulse duration. The simulation shown the result can have 5GHz narrowband width closing to commercial product. Besides, we demonstrated the THz multi-wavelength interference method by using THz-TDS (terahertz time domain spectroscopy) to measure the liquid crystal cell gap. We have also used THz-TDS to investigate the complex optical constants and birefringence of cholesteric liquid crystal mixture BL006. The extraordinary (ne) and ordinary (no) indices of refraction at are 1.784-1.817 and 1.516-1.555 giving rise to a birefringence of 0.25¡V0.29 in 0.2THz~1.6THz.

Doctor of Philosophy / Department of Physics / Zenghu Chang / The few-cycle femtosecond laser pulse has proved itself to be a powerful tool for controlling the electron dynamics inside atoms and molecules. By applying such few-cycle pulses as a driving field, single isolated attosecond pulses can be produced through the high-order harmonic generation process, which provide a novel tool for capturing the real time electron motion. The first part of the thesis is devoted to the state of the art few-cycle near infrared (NIR) laser pulse development, which includes absolute phase control (carrier-envelope phase stabilization), amplitude control (power stabilization), and relative phase control (pulse compression and shaping). Then the double optical gating (DOG) method for generating single attosecond pulses and the attosecond streaking experiment for characterizing such pulses are presented. Various experimental limitations in the attosecond streaking measurement are illustrated through simulation. Finally by using the single attosecond pulses generated by DOG, an attosecond transient absorption experiment is performed to study the autoionization process of argon. When the delay between a few-cycle NIR pulse and a single attosecond XUV pulse is scanned, the Fano resonance shapes of the argon autoionizing states are modified by the NIR pulse, which shows the direct observation and control of electron-electron correlation in the temporal domain.

To capture electronic rearrangements inside a molecule or during chemical reactions, attosecond (as, 1 as =10−18 s) time resolution is needed. To create a light pulse with this duration, the central frequency has to be in the XUV range and cover several tens of eVs. Moreover, the frequency components have to be synchronized. The so called High Harmonic Generation (HHG) in gases well suits this task. During this process a high intensity laser pulse is focused in a gas jet, where its electric field bends the potential barrier of an atom allowing an electron wave packet (EWP) to tunnel ionize. Following the electric field of the laser the EWP gets accelerated, gaining a large kinetic energy that may be released as a high energy (XUV) photon in the event of a re-collision with the ionic core. These recolliding EWP probe the structure and dynamics of the core in a self-probing scheme: the EWP, that is emitted by the molecule at a certain time, probes itself later. More precisely, this "self-probing" scheme gives access to the complex valued recombination dipole moment (RDM) of the molecule which is determined by both the nuclear and electronic structure. The recombination encodes these characteristics into the spectral amplitude, phase and polarization state of the harmonic radiation emitted by the dipole. Due to the coherent nature of HHG it is possible to measure all these three parameters. Moreover, it is in principle possible through a tomographic procedure to reconstruct the radiating orbital.The objective of my thesis was two-fold. By implementing advanced characterization techniques of the harmonic amplitude, phase and polarization we studied i) the electronic structure of N2 and laser induced multi-channel tunnel ionization. We presented the reconstruction of molecular orbitals and revealed the ionization channel dependent ultrafast nuclear vibration. We also studied ii) the reflectivity and dispersion of recently designed chirped XUV mirrors that can shape the temporal profile of attosecond pulses. With these mirrors we could control the spectral phase over 20 eV and compensate the GDD of the harmonics or introduce a TOD. We also proposed a novel attosecond pulse shaper.

In the presented thesis the topic of femtosecond pulse dispersion and methods of characterizing pulse profile are briefly introduced. Then, a functionality of a spatial light modulator is described. The spatial light modulator was used in an experimental scheme called the pulse shaper, which allowed independent amplitude and phase modulation of pulses. Duration and dispersion of pulses was measured by two methods called MIIPS and PICASO. MIIPS was also used for a reconstruction of a spectral phase of pulses. The autocorrelator was constructed on a design of the Mach-Zehnder interferometer. The duration of the shortest measured pulse (13.3 ± 0.5) fs was retrieved from measured interferometric autocorrelations by PICASO. Furthermore, theoretical dependence of pulse duration on the group delay dispersion was confirmed for pulses shorter than 120 fs. The group velocity dispersion was measured for fused silica windows and for a pair of diffraction gratings in the pulse shaper. Both values confirmed theoretical expectations.

This thesis focuses on improving the performance of the THz time-domain spectroscopy system using second-order nonlinear crystals for THz generation and detection in terms of bandwidth, sensitivity, and THz field strength. The theories for the THz generation based on optical rectification and detection technique, electro-optical sampling, based on Pockels effect are introduced in Chapter 2. In Chapter 3, some experiments are presented to characterize the performances of the THz system based on a 180 fs Yb:KGW femtosecond laser amplifier operating at 1035 nm. The Yb-based femtosecond laser is becoming increasingly popular due to its robustness, high repetition rate, and high average power. However, the NIR bandwidth of these femtosecond lasers is limited by the gain bandwidth of the gain medium, and achieving pulse durations shorter than 180 fs is challenging. Consequently, the full bandwidth of THz time-domain spectroscopy systems is constrained by such laser systems. In order to broaden the THz bandwidth of such THz time-domain spectroscopy systems, our work in Chapter 4 combines the Yb:KGW femtosecond laser amplifier with an argon-filled hollow-core photonic crystal fiber pulse shaper to spectrally broaden the near-infrared pulses from 3.5 to 8.7 THz, increasing the measured THz bandwidth correspondingly from 2.3 THz to 4.5 THz. This is one of the first works to have broadband THz system based on Yb-based femtosecond lasers in the year of 2018. In Chapter 5, the tilted-pulse-front phase matching in the THz generation and detection scheme is demonstrated using the same surface-etched phase gratings on the front surfaces of the 2 mm-thick GaP generation and detection crystals. This scheme overcomes the THz generation and detection bandwidth limit of thick crystals imposed by the traditional collinear phase matching, while allowing the long nonlinear interaction length. This results in a THz spectral range from 0.1 to 6.5 THz with a peak at 3 THz and a peak dynamic range of 90 dB. In the range between 1.1 and 4.3 THz, the system dynamic range exceeds 80 dB. Based on this contact grating-based THz generation, the next step involves generating high-field THz above 2 THz. For high-field THz generation, the most renowned technique is the tilted-pulse-front technique, which generates high-field THz below 2 THz in a LiNbO₃ crystal. Most nonlinear optics experiments in the THz regime rely on such THz sources. To generate high-field THz above 2 THz, one promising candidate is organic THz crystals. However, most organic crystals require a pump laser with a wavelength exceeding 1200 nm, necessitating a more complex laser system. Additionally, the low damage threshold of these crystals are susceptible to compromise the stability of the measurements. Other techniques, such as air plasma and metallic spintronics, can generate ultra-broadband high-field THz from 0.1 to 30 THz, but the pulse energy within certain frequency windows is relatively low, rendering these THz sources less effective for nonlinearly driving specific optical transitions. On the other hand, semiconductor crystals as THz generation crystals, have a high damage threshold and can achieve good phase matching at wavelength around 800 or 1000 nm. In Chapter 6, high-field THz generation with a peak field of 303 kV/cm and a spectral peak at 2.6 THz is achieved with a more homogenous grating on the surface of a 1 mm-thick GaP generation crystal in a configuration collimating the near-infrared generation beam with a pulse energy of 0.57 mJ onto the generation crystal. The experiments also show that the system operates significantly below the GaP damage threshold and THz generation saturation regime, indicating that the peak THz field strength can approach 1 MV/cm, with a 5 mJ near-infrared generation pulse. This is the first high-field THz source based on semiconductor crystals capable of generating high-field THz above 2 THz. With such a THz source, we can conduct nonlinear optics experiments above 2 THz, including the study of phonon-assisted nonlinearities, coherent control of Bose-Einstein condensation of excitons and polaritons in semiconductor cavities, and saturable absorption in molecular gases.

Broadband spectral content is required to support ultrashort pulses. However this broadband content is subject to dispersion and hence the pulse duration of corresponding ultrashort pulses may be stretched accordingly. I used a commercially-available adaptive ultrashort pulse shaper featuring multiphoton intrapulse interference phase scan technology to characterise and compensate for the dispersion of the optical system in situ and conducted experimental and theoretical studies in various inter-linked topics relating to the light-matter interaction. Firstly, I examined the role of broadband ultrashort pulses in novel light-matter interacting systems involving optically co-trapped particle systems in which inter-particle light scattering occurs between optically-bound particles. Secondly, I delivered dispersion-compensated broadband ultrashort pulses in a dispersive microscope system to investigate the role of pulse duration in a biological light-matter interaction involving laser-induced cell membrane permeabilisation through linear and nonlinear optical absorption. Finally, I examined some of the propagation characteristics of broadband ultrashort pulse propagation using a computer-controlled spatial light modulator. The propagation characteristics of ultrashort pulses is of paramount importance for defining the light-matter interaction in systems. The ability to control ultrashort pulse propagation by using adaptive dispersion compensation enables chirp-free ultrashort pulses to be used in experiments requiring the shortest possible pulses for a specified spectral bandwidth. Ultrashort pulsed beams may be configured to provide high peak intensities over long propagation lengths, for example, using novel beam shapes such as Bessel-type beams, which has applications in biological light-matter interactions including phototransfection based on laser-induced cell membrane permeabilisation. The need for precise positioning of the beam focus on the cell membrane becomes less strenuous by virtue of the spatial properties of the Bessel beam. Dispersion compensation can be used to control the temporal properties of ultrashort pulses thus permitting, for example, a high peak intensity to be maintained along the length of a Bessel beam, thereby reducing the pulse energy required to permeabilise the cell membrane and potentially reduce damage therein.