We present a new mechanism for high-order harmonic generation by reflection of a laser beam from an overdense plasma, efficient even at moderate laser intensities (down to $I{\lambda }^2\approx 4\times {10}^{15}\mathrm{W}{\mathrm{cm}}^{-2}\mu {\mathrm{m}}^2$). In this mechanism, a transient phase matching between the electromagnetic field and plasma oscillations within a density gradient leads to the emission of harmonics up to the plasma frequency. These plasma oscillations are periodically excited in the wake of attosecond electron bunches which sweep across the density gradient. This process leads to a train of unevenly spaced chirped attosecond pulses and, hence, to broadened and chirped harmonics. This last effect is confirmed experimentally.

Free-electron lasers generate high-brilliance coherent radiation at wavelengths spanning from the infrared to the X-ray domains. The recent development of short-wavelength seeded free-electron lasers now allows for unprecedented levels of control on longitudinal coherence, opening new scientific avenues such as ultra-fast dynamics on complex systems and X-ray nonlinear optics. Although those devices rely on state-of-the-art large-scale accelerators, advancements on laser-plasma accelerators, which harness gigavolt-per-centimetre accelerating fields, showcase a promising technology as compact drivers for free-electron lasers. Using such footprint-reduced accelerators, exponential amplification of a shot-noise type of radiation in a self-amplified spontaneous emission configuration was recently achieved. However, employing this compact approach for the delivery of temporally coherent pulses in a controlled manner has remained a major challenge. Here we present the experimental demonstration of a laser-plasma accelerator-driven free-electron laser in a seeded configuration, where control over the radiation wavelength is accomplished. Furthermore, the appearance of interference fringes, resulting from the interaction between the phase-locked emitted radiation and the seed, confirms longitudinal coherence. Building on our scientific achievements, we anticipate a navigable pathway to extreme-ultraviolet wavelengths, paving the way towards smaller-scale free-electron lasers, unique tools for a multitude of applications in industry, laboratories and universities.

Laser-plasma accelerators can produce high-quality electron beams, up to giga electronvolts in energy, from a centimetre scale device. The properties of the electron beams and the accelerator stability are largely determined by the injection stage of electrons into the accelerator. The simplest mechanism of injection is self-injection, in which the wakefield is strong enough to trap cold plasma electrons into the laser wake. The main drawback of this method is its lack of shot-to-shot stability. Here we present experimental and numerical results that demonstrate the existence of two different self-injection mechanisms. Transverse self-injection is shown to lead to low stability and poor-quality electron beams, because of a strong dependence on the intensity profile of the laser pulse. In contrast, longitudinal injection, which is unambiguously observed for the first time, is shown to lead to much more stable acceleration and higher-quality electron beams.