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Laser-driven plasma accelerators can produce high-energy, high peak current ion beams by irradiating solid materials with ultra-intense laser pulses. This innovative concept attracts a lot of attention for various multidisciplinary applications as a compact and energy-efficient alternative to conventional accelerators. The maturation of plasma accelerators from complex physics experiments to turnkey particle sources for practical applications necessitates breakthroughs in the generated beam parameters, their robustness and scalability to higher repetition rates and efficiencies. This thesis investigates viable optimisation strategies for enhancing ion acceleration from thin foil targets in ultra-intense laser-plasma interactions. The influence of the detailed laser pulse parameters on plasma-based ion acceleration has been systematically investigated in a series of experiments carried out on two state-of-the-art high-power laser systems. A central aspect of this work is the establishment and integration of laser diagnostics and operational techniques to advance control of the interaction conditions for maximum acceleration performance. Meticulous efforts in continuously monitoring and enhancing the temporal intensity contrast of the laser system, enabled to optimise ion acceleration in two different regimes, each offering unique perspectives for applications. Using the widely established target-normal sheath acceleration (TNSA) scheme and adjusting the temporal shape of the laser pulse accordingly, proton energies up to 70 MeV were reliably obtained over many months of operation. Asymmetric laser pulses, deviating significantly from the standard conditions of an ideally compressed pulse, resulted in the highest particle numbers and an average energy gain ≥ 37 %. This beam quality enhancement is demonstrated across a broad range of parameters, including thickness and material of the target, laser energy and temporal intensity contrast. To overcome the energy scaling limitations of TNSA, the second part of the thesis focuses on an advanced acceleration scheme occurring in the relativistically induced transparency (RIT) regime. The combination of thin foil targets with precisely matched temporal contrast conditions of the laser enabled a transition of the initially opaque targets to transparency upon main pulse arrival. Laser-driven proton acceleration to a record energy of 150 MeV is experimentally demonstrated using only 22 J of laser energy on target. The low-divergent high-energy component of the accelerated beam is spatially and spectrally well separated from a lower energetic TNSA component. Start-to-end simulations validate these results and elucidate the role of preceding laser light in pre-expanding the target along with the detailed acceleration dynamics during the main pulse interaction. The ultrashort pulse duration of the laser facilitates a rapid succession of multiple known acceleration regimes to cascade efficiently at the onset of RIT, leading to the observed beam parameters and enabling ion acceleration to unprecedented energies. The discussed acceleration scheme was successfully replicated at two different laser facilities and for different temporal contrast levels. The results demonstrate the robustness of this scenario and that the optimum target thickness decreases with improved laser contrast due to reduced pre-expansion. Target transparency was found to identify the best-performance shots within the acquired data sets, making it a suitable feedback parameter for automated laser and target optimisation to enhance stability of plasma accelerators in the future. Overall, the obtained results and described optimisation strategies of this thesis may become the guiding step for the further development of laser-driven ion accelerators.:1 Introduction 1.1 Motivation 1.2 Thesis outline 2 Fundamentals of laser-matter interactions 2.1 Plasma 2.1.1 Plasma properties 2.1.2 Dispersion relation of a plasma 2.1.3 Laser propagation in a plasma 2.2 Laser-matter interactions 2.2.1 Ionisation processes 2.2.2 Electron dynamics in the laser field 2.2.3 Ponderomotive force 2.2.4 Plasma heating processes 2.3 Laser-driven ion acceleration mechanisms 2.3.1 Target normal sheath acceleration 2.3.2 Radiation pressure acceleration 2.3.3 Acceleration in the relativistically induced transparency regime 3 Methodology for high-power laser experiments 3.1 High-power lasers 3.1.1 High-power laser techniques 3.1.2 Temporal contrast of high-power laser systems 3.1.3 DRACO laser system 3.1.4 J-KAREN-P laser system 3.2 Experimental Area 3.2.1 Short-f chamber at HZDR 3.2.2 Short-f chamber at KPSI 3.3 Targets 3.4 Optical diagnostic 3.4.1 Transmitted and reflected laser light 3.4.2 Spectral phase measurements 3.5 Particle diagnostic 3.5.1 Thomson parabola spectrometer 3.5.2 Time of flight measurements 3.5.3 Spatial proton beam profiler 3.5.4 Radiochromic films 3.5.5 Nuclear activation measurements 4 Optimisation of sheath acceleration for high-quality proton beams 4.1 Introduction 4.2 Temporal contrast at experimental environment 4.3 Plasma mirror 4.3.1 Plasma mirror implementation at DRACO-PW 4.3.2 Plasma mirror characterisation at DRACO-PW 4.4 Temporal pulse shaping by spectral phase modification 4.4.1 Theory on temporal pulse shaping 4.4.2 Experimental realisation and results 4.5 Proton acceleration under optimised temporal contrast conditions 4.6 Experimental results 4.7 Discussion on numerical simulations 4.8 Conclusions 5 Enhanced ion acceleration in the relativistic transparency regime 5.1 Introduction 5.2 Experimental setup using the J-KAREN-P laser 5.3 Experimental results 5.4 Laser-induced breakdown and target pre-expansion 5.5 Elucidating ion acceleration in the relativistically induced transparency regime 5.5.1 Details on simulation methodology 5.5.2 Simulation results 5.6 Acceleration in the RIT regime for modified temporal contrast 5.6.1 Experimental setup using the DRACO-PW laser 5.6.2 Experimental results using the DRACO-PW laser 5.6.3 Simulation results for modified temporal contrast 5.7 Conclusions 6 Ion acceleration beyond the 100 MeV frontier from cascading acceleration schemes 6.1 Introduction 6.2 Experimental setup 6.3 Experimental results 6.3.1 Analysis of acceleration performance 6.3.2 Spatial proton beam profile 6.3.3 Nuclear activation measurement 6.3.4 Scaling of maximum proton energy 6.4 Numerical simulations 6.4.1 Simulation setup 6.4.2 Simulation results & discussion 6.5 Conclusions 7 Summary and outlook Appendix References

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