Development of compact electron accelerators and free-electron lasers requires novel acceleration schemes at shorter driving wavelengths. The Axsis project seeks to developterahertz based electron acceleration as well as the high energy terahertz sources required. This thesis explores the methods and optical material required for the generation of highenergymulti-cycle terahertz pulses. Two experimental concepts to generate high energy terahertz radiation are presented. In addition the theoretical background and the optical properties of pertinent optical materials in the terahertz range are discussed. Investigations of the materials are performed with a terahertz time domain spectrometer and a Fourier transform infrared spectrometer. The nonlinear optical crystal lithium niobate as well as other crystals suitable for the terahertz generation and in addition polymers and other radiation attenuators are characterized in the range from 0.2 to 1 THz. The theory describing the generation of narrowband terahertz radiation is evaluated. The experimental setups to generate terahertz radiation and to characterize its properties are described. The specific crystals (periodically poled lithium niobate (PPLN)) used in the experiments to generate the multi-cycle terahertz radiation are examined to determine e.g. the poling period. The first experimental concept splits the ultra fast, broadband pump pulses into a pulse train in order to pump the PPLN at a higher uence while increasing the damage limit. The measurements confirm that a pulse train of ultra short, broadband pump pulses increases not only the terahertz energy but also the energy conversion efficiency. The second experimental concept utilizes chirped and delayed infrared laser pulses. This pulse format makes it possible to pump the crystal with high energy pulses resulting in high energy terahertz radiation. The concept is optimized to reach energies up to 127 μJ exceeding the existing results of narrowband terahertz sources by two orders of magnitude. These results endorse the proposed methods of generating multi-cycle THz pulses at the mJ-level and show a pathway for further scaling to the multi-mJ-level required for theconstruction of the electron accelerator in the Axsis project
