In this thesis we have utilized few-cycle pulses in the range 10-15s, to initiate CE to allow us to image the structure, dynamics, and kinetics of ionization and dissociation of triatomic molecules. We have made a series of measurements of this process for CO2 and N2O, by varying the laser pulse duration from 7 to 500 fs with intensity ranging from 2.5×1014 to 4×1015 (W/cm2), in order to identify the charge states and time scales involved. This is a new approach in CEI introducing a multi-dimensional aspect to the science of non-perturbative laser-molecule interaction. We refer to this approach as FEmtosecond Multi-PUlse Length Spectroscopy (FEMPULS). The use of a time and position sensitive detector allow us to observe all fragment ions in coincidence. By representing the final fragmentation with Dalitz and Newton plots, we have identified the underlying break up dynamics. Momentum conservation has been used to extract the correlated fragment ions which come from a single parent ion. This is achieved by considering that the total momentum of all correlated fragments must add up to zero. One of the main outcomes of our study is observation of charge resonance enhanced ionization (CREI) for triatomic molecules. In the case of CO2, we found that for the 4+ and higher charge states, 100 fs is the time scale required to reach the critical geometry RCO= 2.1Å and ӨOCO =163º (equilibrium CO2 geometry is RCO= 1:16Å and ӨOCO =172º. The CO23+ molecule, however, appears always to begin dissociation from closer than 1.7 Å indicating that dynamics on charge states lower than 3+ is not sufficient to initiate CREI. Finally, we make quantum ab initio calculations of ionization rates for CO2 and identify the electronic states responsible for CREI. Total kinetic energy (KER) has been measured for channels (1, 1, 1) to (2, 2, 2) and it was found that the (1, 1, 1) channel is not Coulombic, while (2, 2, 2) channel is very close to Coulombic (KER close to 90% of the coulombic potential). As another outcome of our study, for the case of N2O, we observed for the first time that there are two stepwise dissociation pathways for N2O3+: (1) N2O3+ → N++ NO2+ → N+ + N++ O+ and (2) N2O3+ → N22++O+ → N+ + N++ O+ as well as one for N2O4+ → N2++ NO2+ → N2+ + N++ O+. The N22+ stepwise channel is suppressed for longer pulse length, a phenomenon which we attribute to the influence which the structure of the 3+ potential has on the dissociating wave packet propagation. Finally, by observing the KER for each channel as a function of pulse duration, we show the increasing importance of CREI for channels higher than 3+.

The ultrashort chirped pulse amplification (CPA) laser technology opens the path to high intensities of 10^21 W/cm² and above in the laser focus. Such intensities allow laser-matter interaction in the relativistic intensity regime. Direct diode-pumped ultrashort solid-state lasers combine high-energy, high-power and efficient amplification together, which are the main advantages compared to flashlamp-pumped high-energy laser systems based on titanium-doped sapphire. Development within recent years in the field of laser diodes makes them more and more attractive in terms of total costs, compactness and lifetime. This work is dedicated to the Petawatt, ENergy-Efficient Laser for Optical Plasma Experiments (PENELOPE) project, a fully and directly diode-pumped laser system under development at the Helmholtz–Zentrum Dresden – Rossendorf (HZDR), aiming at 150 fs long pulses with energies of up to 150 J at repetition rates of up to 1 Hz. The focus of this thesis lies on the spectral and width manipulation of the front-end amplifiers, trivalent ytterbium-doped calcium fluoride (Yb3+:CaF2) as gain material as well as the pump source for the final two main amplifiers of the PENELOPE laser system. Here, all crucial design parameters were investigated and a further successful scaling of the laser system to its target values was shown. Gain narrowing is the dominant process for spectral bandwidth reduction during the amplification at the high-gain front-end amplifiers. Active or passive spectral gain control filter can be used to counteract this effect. A pulse duration of 121 fs was achieved by using a passive spectral attenuation inside a regenerative amplifier, which corresponds to an improvement by a factor of almost 2 compared to the start of this work. A proof-of-concept experiment showed the capability of the pre-shaping approach. A spectral bandwidth of 20nm was transferred through the first multipass amplifier at a total gain of 300. Finally, the predicted output spectrum calculated by a numerical model of the final amplifier stages was in a good agreement with the experimental results. The spectroscopic properties of Yb3+:CaF2 matches the constraints for ultrashort laser pulse amplification and direct diode pumping. Pumping close to the zero phonon line at 976nm is preferable compared to 940nm as the pump intensity saturation is significantly lower. A broad gain cross section of up to 50nm is achievable for typical inversion levels. Furthermore, moderate cryogenic temperatures (above 200K) can be used to improve the amplification performance of Yb3+:CaF2. The optical quality of the doped crystals currently available on the market is sufficient to build amplifiers in the hundred joule range. The designed pump source for the last two amplifiers is based on two side pumping in a double pass configuration. However, this concept requires the necessity of brightness conservation for the installed laser diodes. Therefore, a fully relay imaging setup (4f optical system) along the optical path from the stacks to the gain material including the global beam homogenization was developed in a novel approach. Beside these major parts the amplifier architecture and relay imaging telescopes as well as temporal intensity contrast (TIC) was investigated. An all reflective concept for the relay imaging amplifiers and telescopes was selected, which results in several advantages especially an achromatic behavior and low B-Integral. The TIC of the front-end was improved, as the pre- and postpulses due to the plane-parallel active-mirror was eliminated by wedging the gain medium.

The ultrashort chirped pulse amplification (CPA) laser technology opens the path to high intensities of 10^21 W/cm² and above in the laser focus. Such intensities allow laser-matter interaction in the relativistic intensity regime. Direct diode-pumped ultrashort solid-state lasers combine high-energy, high-power and efficient amplification together, which are the main advantages compared to flashlamp-pumped high-energy laser systems based on titanium-doped sapphire. Development within recent years in the field of laser diodes makes them more and more attractive in terms of total costs, compactness and lifetime. This work is dedicated to the Petawatt, ENergy-Efficient Laser for Optical Plasma Experiments (PENELOPE) project, a fully and directly diode-pumped laser system under development at the Helmholtz–Zentrum Dresden – Rossendorf (HZDR), aiming at 150 fs long pulses with energies of up to 150 J at repetition rates of up to 1 Hz. The focus of this thesis lies on the spectral and width manipulation of the front-end amplifiers, trivalent ytterbium-doped calcium fluoride (Yb3+:CaF2) as gain material as well as the pump source for the final two main amplifiers of the PENELOPE laser system. Here, all crucial design parameters were investigated and a further successful scaling of the laser system to its target values was shown. Gain narrowing is the dominant process for spectral bandwidth reduction during the amplification at the high-gain front-end amplifiers. Active or passive spectral gain control filter can be used to counteract this effect. A pulse duration of 121 fs was achieved by using a passive spectral attenuation inside a regenerative amplifier, which corresponds to an improvement by a factor of almost 2 compared to the start of this work. A proof-of-concept experiment showed the capability of the pre-shaping approach. A spectral bandwidth of 20nm was transferred through the first multipass amplifier at a total gain of 300. Finally, the predicted output spectrum calculated by a numerical model of the final amplifier stages was in a good agreement with the experimental results. The spectroscopic properties of Yb3+:CaF2 matches the constraints for ultrashort laser pulse amplification and direct diode pumping. Pumping close to the zero phonon line at 976nm is preferable compared to 940nm as the pump intensity saturation is significantly lower. A broad gain cross section of up to 50nm is achievable for typical inversion levels. Furthermore, moderate cryogenic temperatures (above 200K) can be used to improve the amplification performance of Yb3+:CaF2. The optical quality of the doped crystals currently available on the market is sufficient to build amplifiers in the hundred joule range. The designed pump source for the last two amplifiers is based on two side pumping in a double pass configuration. However, this concept requires the necessity of brightness conservation for the installed laser diodes. Therefore, a fully relay imaging setup (4f optical system) along the optical path from the stacks to the gain material including the global beam homogenization was developed in a novel approach. Beside these major parts the amplifier architecture and relay imaging telescopes as well as temporal intensity contrast (TIC) was investigated. An all reflective concept for the relay imaging amplifiers and telescopes was selected, which results in several advantages especially an achromatic behavior and low B-Integral. The TIC of the front-end was improved, as the pre- and postpulses due to the plane-parallel active-mirror was eliminated by wedging the gain medium.