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Particle accelerators driven by laser-generated terahertz (THz) pulses promise unprecedented control over the energy–time phase space of particle bunches compared with conventional radiofrequency technology. Here we demonstrate acceleration of a relativistic electron beam in a THz-driven linear accelerator. Narrowband THz pulses were tuned to the phase-velocity-matched operating frequency of a rectangular dielectric-lined waveguide for extended collinear interaction with 35 MeV, 60 pC electron bunches, imparting multicycle energy modulation to chirped (6 ps) bunches and injection phase-dependent energy gain (up to 10 keV) to subcycle (2 ps) bunches. These proof-of-principle results establish a route to whole-bunch linear acceleration of subpicosecond particle beams, directly applicable to scaled-up and multistaged concepts capable of preserving beam quality, thus marking a key milestone for future THz-driven acceleration of relativistic beams.Relativistic 35 MeV electron bunches with charges of 60 pC are accelerated in a terahertz-wave-driven dielectric waveguide. When the terahertz pulse energy is 0.8 μJ, an accelerating gradient of 2 MeV m−1 and energy gain of 10 keV are achieved.

Laser-plasma wakefield acceleration (LWFA) offers ultrahigh accelerating gradients in compact setups, but the complex non-linear nature of the process makes it challenging to generate high-quality beams. Injection of electron bunches from an external source into a plasma accelerator provides a promising route to improved performance; however, electron bunches from conventional radio-frequency (RF)-based injectors suffer from non-linear compression and laser-beam asynchrony, leading to energy jitter and emittance growth. We present a fundamental concept of terahertz-controlled electron bunches for external injection into LWFA. This terahertz-frequency approach provides temporal locking between the electron beam and the drive laser, and enables the compression of high-quality beams to sub-10-fs durations before injection into the LWFA. Numerical simulations demonstrate that GeV-scale acceleration with excellent beam quality and stability -- energy jitter and energy spread around 0.2% -- can be achieved using this method. This concept opens new opportunities for stable, multi-stage laser-driven accelerators and supports the development of next-generation applications such as free-electron lasers (FELs).

We demonstrate that narrowband multi-cycle terahertz (MC-THz) sources based on periodically-poled lithium niobate (PPLN) wafer stacks can be driven by high repetition-rate, high energy femtosecond ytterbium-doped lasers. Operating at 10-kHz repetition rate with up to 104 W of pump power on a 10-wafer stack, we measure 26.4 mW of THz average power for a narrowband multi-cycle source. We identify and quantify strong lensing effects causing dramatic beam focusing in 47 wafer stacks which act as a primary limitation in the current configuration, and present mitigation strategies for future scaling. This first study of high average power narrowband multi-cycle THz sources offers a path forward to Watt-level high repetition rate sources using thin lithium niobate plates.

Femtosecond relativistic electron bunches and micro-bunch trains synchronised with femtosecond precision to external laser sources are widely sought for next-generation accelerator and photonic technologies, from extreme UV and X-ray light sources for materials science, to ultrafast electron diffraction and future high-energy physics colliders. While few-femtosecond bunches have been demonstrated, achieving the control, stability and femtosecond-level laser synchronisation remains critically out of reach. Here we demonstrate a concept for laser-driven compression of high-energy (35.5 MeV) electron bunches with temporal synchronisation to a high-power (few-TW) laser system. Laser-generated multi-cycle terahertz (THz) pulses drive periodic electron energy modulation, enabling subsequent magnetic compression capable of generating tuneable picosecond-spaced bunch trains with 30 pC total charge and 50 A peak currents, or to compress a single bunch by a factor of 27 down to 15 fs duration. The THz-driven compression simultaneously drives temporal-locking of the bunch to the THz drive laser, providing a route to femtosecond-level synchronisation, overcoming the timing jitter inherent to radio-frequency accelerators and high-power laser systems. This THz technique offers compact and flexible bunch control with unprecedented temporal synchronisation, opening a pathway to unlock new capabilities for free electron lasers, ultrafast electron diffraction and novel plasma accelerators.

Dielectric structures driven by laser-generated terahertz (THz) pulses may hold the key to overcoming the technological limitations of conventional particle accelerators and with recent experimental demonstrations of acceleration, compression and streaking of low-energy (sub-100 keV) electron beams, operation at relativistic beam energies is now essential to realize the full potential of THz-driven structures. We present the first THz-driven linear acceleration of relativistic 35 MeV electron bunches, exploiting the collinear excitation of a dielectric-lined waveguide driven by the longitudinal electric field component of polarization-tailored, narrowband THz pulses. Our results pave the way to unprecedented control over relativistic electron beams, providing bunch compression for ultrafast electron diffraction, energy manipulation for bunch diagnostics, and ultimately delivering high-field gradients for compact THz-driven particle acceleration.

The work in this thesis was submitted to The University of Manchester for the degree of Doctor of Philosophy in September 2016 by Morgan Timothy Hibberd and is entitled \"Studying low frequency vibrational modes using ultrafast techniques\".In this thesis, I report on the investigation of the low frequency vibrational modes in a number of different systems using ultrafast spectroscopic techniques. These consist of biological systems, including the enzyme, morphinone reductase (MR) and the related biomolecules, riboflavin (Rb) and flavin mononucleotide (FMN), as well as non-biological systems, including the semiconductor gallium nitride (GaN) and gold nanoparticles (Au NPs). The term low frequency refers to terahertz (THz) frequencies, where vibrational modes exist at the molecular level, with molecular rotations, lattice vibrations and inter- and intra-molecular vibrations occurring in the THz spectral range. These vibrational modes occur on sub-picosecond timescales and therefore ultrafast techniques utilising femtosecond laser pulses provide a means of studying these modes, and are employed throughout this thesis.The two ultrafast techniques of transient absorption (TA) spectroscopy and terahertz time-domain spectroscopy (THz-TDS) were used. Firstly, a high-repetition rate transient absorption (HRRTA) spectrometer was commissioned to perform pump-probe measurements with an ultraviolet pump and broadband visible probe. The performance of the HRRTA spectrometer was benchmarked using Au NPs and used to investigate the existence of a promoting vibration in MR contributing to the catalysis process, predicted to occur at THz frequencies. Weak oscillations were detected in the charge-transfer absorption band of MR bound to the non-reactive cofactor 1,4,5,6-tetra-hydro-nicotinamide adenine dinucleotide (NADH4), with a frequency of approximately 1.5 THz and provide evidence of the first direct observation of a promoting vibration in an enzyme.To complement the TA measurements, THz-TDS was also used to obtain direct measurements of the absorption at THz frequencies. Due to the challenge of studying water-based biological samples, an initial investigation was performed on a wurtzite GaN wafer, which exhibited optical phonon modes in the THz frequency range that were found to determine the dielectric response of the semi-insulating semiconductor wafer. Use of a non-polar m-plane wafer allowed the anisotropic nature to be observed and values of 9.22 ± 0.02 and 10.32 ± 0.03 for the static dielectric constants were obtained for the THz electric field polarised both perpendicular and parallel to the c-axis of the wurtzite GaN wafer, respectively. Finally, biological studies using THz-TDS were performed with measurements on Rb pellets and films revealing vibrational modes in the THz region. The sharp absorption features were not observed in FMN, despite a small difference in molecular content from Rb, and dehydration was required to reveal small amplitude absorption features. Final measurements on MR and MR-NADH4 films were carried out and evidence of absorption features in the THz frequency range were observed, however further work is required to determine the precise origin of these features.