Laser-plasma accelerators (LPAs) are capable of accelerating charged particles to very high energies in very compact structures. In theory, therefore, they offer advantages over conventional, large-scale particle accelerators. However, the energy gain in a single-stage LPA can be limited by laser diffraction, dephasing, electron-beam loading and laser-energy depletion. The problem of laser diffraction can be addressed by using laser-pulse guiding and preformed plasma waveguides to maintain the required laser intensity over distances of many Rayleigh lengths; dephasing can be mitigated by longitudinal tailoring of the plasma density; and beam loading can be controlled by proper shaping of the electron beam. To increase the beam energy further, it is necessary to tackle the problem of the depletion of laser energy, by sequencing the accelerator into stages, each powered by a separate laser pulse. Here, we present results from an experiment that demonstrates such staging. Two LPA stages were coupled over a short distance (as is needed to preserve the average acceleration gradient) by a plasma mirror. Stable electron beams from a first LPA were focused to a twenty-micrometre radius--by a discharge capillary-based active plasma lens--into a second LPA, such that the beams interacted with the wakefield excited by a separate laser. Staged acceleration by the wakefield of the second stage is detected via an energy gain of 100 megaelectronvolts for a subset of the electron beam. Changing the arrival time of the electron beam with respect to the second-stage laser pulse allowed us to reconstruct the temporal wakefield structure and to determine the plasma density. Our results indicate that the fundamental limitation to energy gain presented by laser depletion can be overcome by using staged acceleration, suggesting a way of reaching the electron energies required for collider applications.

Acceleration and manipulation of electron bunches underlie most electron and X-ray devices used for ultrafast imaging and spectroscopy. New terahertz-driven concepts offer orders-of-magnitude improvements in field strengths, field gradients, laser synchronization and compactness relative to conventional radio-frequency devices, enabling shorter electron bunches and higher resolution with less infrastructure while maintaining high charge capacities (pC), repetition rates (kHz) and stability. We present a segmented terahertz electron accelerator and manipulator (STEAM) capable of performing multiple high-field operations on the 6D-phase-space of ultrashort electron bunches. With this single device, powered by few-micro-Joule, single-cycle, 0.3 THz pulses, we demonstrate record THz-acceleration of >30 keV, streaking with <10 fs resolution, focusing with >2 kT/m strength, compression to ~100 fs as well as real-time switching between these modes of operation. The STEAM device demonstrates the feasibility of THz-based electron accelerators, manipulators and diagnostic tools enabling science beyond current resolution frontiers with transformative impact.

T abletop plasma accelerators can now produce GeV-range electron beams 1-5 and femtosecond X-ray pulses 6 , providing compact radiation sources for medicine, nuclear engineering, materials science and high-energy physics 7 . In these accelerators, electrons surf on electric fields exceeding 100 GeV m −1 , which is more than 1,000 times stronger than achievable in conventional accelerators. These fields are generated within plasma structures (such as Langmuir waves 8 or electron density 'bubbles' 9 ) propagating near light speed behind laser 2-4 or charged-particle 5 driving pulses. Here, we demonstrate single-shot visualization of laser-wakefield accelerator structures for the first time. Our 'snapshots' capture the evolution of multiple wake periods, detect structure variations as laser-plasma parameters change, and resolve wavefront curvature; features never previously observed.These previously invisible features underlie wave breaking, electron injection and focusing within the wake, the key determinants of charge, energy, energy spread and collimation of the accelerated beam. Because of their microscopic size and luminal velocity, these critical structures previously eluded direct singleshot observation, inhibiting progress in producing high-quality beams and in correlating beam properties with wake structure. Here, in contrast, we reconstruct wake morphology in real-time, enabling rapid feedback and optimization.Recent advances in laser-wakefield accelerators dramatically illustrated the link between beam quality and plasma structure 1-4 . Earlier laser-wakefield accelerators produced electron beams with large divergence and energy spread, but by introducing a plasma channel guide 1,2 or by carefully adjusting the laser-plasma conditions to produce an electron density cavity behind the driving pulse 3,4 , collimated, nearly mono-energetic beams from 80 MeV to 1 GeV were demonstrated. Nevertheless, the plasma structures themselves remained invisible. Previous direct measurements of laser wakes with spatial resolution better than a plasma wavelength 10-13 (l p ) used frequency-domain interferometry 14 , in which a focused femtosecond probe pulse measured local electron density n e (ζ) at only a single time delay ζ behind the driving pulse within the co-propagating wake for each laser shot. Wake structure was then accumulated painstakingly by probing a different ζ on each subsequent shot. However, multi-shot techniques average over

X-ray spectroscopy is used to obtain single-shot information on electron beam emittance in a low-energy-spread 0.5 GeV-class laser-plasma accelerator. Measurements of betatron radiation from 2 to 20 keV used a CCD and single-photon counting techniques. By matching x-ray spectra to betatron radiation models, the electron bunch radius inside the plasma is estimated to be ~0.1 μm. Combining this with simultaneous electron spectra, normalized transverse emittance is estimated to be as low as 0.1 mm mrad, consistent with three-dimensional particle-in-cell simulations. Correlations of the bunch radius with electron beam parameters are presented.

Compact, tunable, radially symmetric focusing of electrons is critical to laser-plasma accelerator (LPA) applications. Experiments are presented demonstrating the use of a discharge-capillary active plasma lens to focus 100-MeV-level LPA beams. The lens can provide tunable field gradients in excess of 3000 T/m, enabling cm-scale focal lengths for GeV-level beam energies and allowing LPA-based electron beams and light sources to maintain their compact footprint. For a range of lens strengths, excellent agreement with simulation was obtained.

X-ray crystallography is one of the main methods to determine atomic-resolution 3D images of the whole spectrum of molecules ranging from small inorganic clusters to large protein complexes consisting of hundred-thousands of atoms that constitute the macromolecular machinery of life. Life is not static, and unravelling the structure and dynamics of the most important reactions in chemistry and biology is essential to uncover their mechanism. Many of these reactions, including photosynthesis which drives our biosphere, are light induced and occur on ultrafast timescales. These have been studied with high time resolution primarily by optical spectroscopy, enabled by ultrafast laser technology, but they reduce the vast complexity of the process to a few reaction coordinates. In the AXSIS project at CFEL in Hamburg, funded by the European Research Council, we develop the new method of attosecond serial X-ray crystallography and spectroscopy, to give a full description of ultrafast processes atomically resolved in real space and on the electronic energy landscape, from co-measurement of X-ray and optical spectra, and X-ray diffraction. This technique will revolutionize our understanding of structure and function at the atomic and molecular level and thereby unravel fundamental processes in chemistry and biology like energy conversion processes. For that purpose, we develop a compact, fully coherent, THz-driven atto-second X-ray source based on coherent inverse Compton scattering off a free-electron crystal, to outrun radiation damage effects due to the necessary high X-ray irradiance required to acquire diffraction signals. This highly synergistic project starts from a completely clean slate rather than conforming to the specifications of a large free-electron laser (FEL) user facility, to optimize the entire instrumentation towards fundamental measurements of the mechanism of light absorption and excitation energy transfer. A multidisciplinary team formed by laser-, accelerator,- X-ray scientists as well as spectroscopists and biochemists optimizes X-ray pulse parameters, in tandem with sample delivery, crystal size, and advanced X-ray detectors. Ultimately, the new capability, attosecond serial X-ray crystallography and spectroscopy, will be applied to one of the most important problems in structural biology, which is to elucidate the dynamics of light reactions, electron transfer and protein structure in photosynthesis.

Optical second-harmonic generation (SHG) is used as a noninvasive probe of the interfaces of Si nanocrystals (NCs) embedded uniformly in an SiO2 matrix. Measurements of the generated SH mode verify that the second-harmonic polarization has a nonlocal dipole form proportional to (E x Delta inverted) E that depends on inhomogeneities in the incident field E, as proposed in recent models based on a locally noncentrosymmetric dipolar response averaged over the spherical NC interfaces. A two-beam SHG geometry is found to enhance this polarization greatly compared to single-beam SHG, yielding strong signals useful for scanning, spectroscopy, and real-time monitoring. This configuration provides a general strategy for enhancing the second-order nonlinear response of centrosymmetric samples, as demonstrated here for both Si nanocomposites and their glass substrates.

Highly-efficient optical generation of narrowband terahertz radiation enables unexplored technologies and sciences from compact electron acceleration to charge manipulation in solids. State-of-the-art conversion efficiencies are currently achieved using difference-frequency generation driven by temporal beating of chirped pulses but remain, however, far lower than desired or predicted. Here we show that high-order spectral phase fundamentally limits the efficiency of narrowband difference-frequency generation using chirped-pulse beating and resolve this limitation by introducing a novel technique based on tuning the relative spectral phase of the pulses. For optical terahertz generation, we demonstrate a 13-fold enhancement in conversion efficiency for 1%-bandwidth, 0.361 THz pulses, yielding a record energy of 0.6 mJ and exceeding previous optically-generated energies by over an order of magnitude. Our results prove the feasibility of millijoule-scale applications like terahertz-based electron accelerators and light sources and solve the long-standing problem of temporal irregularities in the pulse trains generated by interfering chirped pulses.