Precise parameter control of multicycle terahertz generation in PPLN using flexible pulse trains.

The low (sub %) efficiencies so-far demonstrated for nonlinear optical down-conversion to terahertz (THz) frequencies are a primary limiting factor in the generation of high-energy, high-field THz-radiation pulses (in particular narrowband, multicycle pulses) needed for many scientific fields. However, simulations predict that far higher conversion efficiencies are possible by use of suitably-optimized optical sources. Here we implement a customized optical laser system producing highly-tunable trains of infrared pulses and systematically explore the experimental optimization of the down-conversion process. Our setup, which allows tuning of the energy, duration, number and periodicity of the pulses in the train, provides a unique capability to test predictions of analytic theory and simulation on the parameter dependences for the optical-to-THz difference-frequency generation process as well as to map out, with unprecedented precision, key properties of the nonlinear crystal medium. We discuss the agreements and deviations between simulation and experimental results which, on the one hand, shed light on limitations of the existing theory, and on the other hand, provide the first steps in a recipe for development of practical, high-field, efficiency-optimized THz sources.

Highly efficient generation of narrowband terahertz radiation driven by a two-spectral-line laser in PPLN.

We demonstrate record ∼0.9% efficiencies for optical conversion to narrowband (<1% relative bandwidth) terahertz (THz) radiation by strongly cascaded difference frequency generation. These results are achieved using a novel, to the best of our knowledge, laser source, customized for high efficiencies, with two narrow spectral lines of variable separation and pulse duration (≥250 ps). THz radiation generation in 5% MgO-doped periodically poled lithium niobate (PPLN) crystals of varying poling period was explored at cryogenic and room temperature operation as well as with different crystal lengths. This work addresses an increasing demand for high-field THz radiation pulses which has, up to now, been largely limited by low optical-to-THz radiation conversion efficiencies.

Frequency-comb-based laser system producing stable optical beat pulses with picosecond durations suitable for high-precision multi-cycle terahertz-wave generation and rapid detection.

We generate temporally modulated optical pulses with a beat frequency of 255 GHz, a duration of 360 ps, and a repetition rate of 2 MHz. The temporal envelope, beat frequency, and repetition rate are computer-programmable. A frequency comb serves as a phase and frequency reference for the locking of two laser lines. The system enables beat frequencies that are adjustable in steps of the frequency comb's repetition rate and exhibit Hz-level precision and accuracy. We expect the optical beat pulses to be well suited for versatile multi-cycle terahertz-wave generation with controllable carrier-envelope phase. We demonstrate that the inherent synchronization of the frequency comb's ultra-short pulse train and the synthesized optical beat (or later the multi-cycle terahertz) pulses enables rapid and phase-sensitive sampling of such pulses.

Cascaded interactions mediated by terahertz radiation.

We investigate a regime of parametric amplification in which the pump and signal waves are spectrally separated by only a few hundreds of GHz frequency - therefore resulting in a sub-THz frequency idler wave. Operating in this regime we find an optical parametric amplifier (OPA) behavior which is highly dissimilar to conventional OPAs. In this regime, we observe multiple three-wave mixing processes occurring simultaneously which results in spectral cascading around the pump and signal wave. Via numerical simulations, we elucidate the processes at work and show that cascaded optical parametric amplification offers a pathway toward THz-wave generation beyond the Manly-Rowe limit and toward the generation of high-energy, sparse frequency-combs.

Excitation and Control of Plasma Wakefields by Multiple Laser Pulses.

We demonstrate experimentally the resonant excitation of plasma waves by trains of laser pulses. We also take an important first step to achieving an energy recovery plasma accelerator by showing that a plasma wave can be damped by an out-of-resonance trailing laser pulse. The measured laser wakefields are found to be in excellent agreement with analytical and numerical models of wakefield excitation in the linear regime. Our results indicate a promising direction for achieving highly controlled, GeV-scale laser-plasma accelerators operating at multikilohertz repetition rates.

Analysis of sinusoidally modulated chirped laser pulses by temporally encoded spectral shifting.

We present an analytical formalism elucidating how information is stored in chirped optical probes by describing the effects of sinusoidal temporal modulations on the electric field. We show that the modulations produce spectral sidebands which can be interpreted as temporal sidebands due to the time-wavelength mapping, an effect we call temporally encoded spectral shifting (TESS). A derivation is presented for the case of chirped-pulse spectral interferometry showing how to recover both the amplitude and the periodicity of the modulation from a Fourier transform of the interferogram. The TESS effect, which provides an intuitive picture for interpreting pump-probe experiments with chirped pulses, is illustrated for probing wakefields from a laser-plasma accelerator.

Multistage coupling of independent laser-plasma accelerators.

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.

AXSIS: Exploring the frontiers in attosecond X-ray science, imaging and spectroscopy.

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.

Active Plasma Lensing for Relativistic Laser-Plasma-Accelerated Electron Beams.

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.

Measured bremsstrahlung photonuclear production of 99Mo ((99m)Tc) with 34 MeV to 1.7 GeV electrons.

(99)Mo photonuclear yield was measured using high-energy electrons from Laser Plasma Accelerators and natural molybdenum. Spectroscopically resolved electron beams allow comparisons to Monte Carlo calculations using known (100)Mo(γ,n)(99)Mo cross sections. Yields are consistent with published low-energy data, and higher energy data are well predicted from the calculations. The measured yield is (15±2)×10(-5) atoms/electron (0.92±0.11 GBq/µA) for 25 mm targets at 33.7 MeV, rising to (1391±20)×10(-5) atoms/electron (87±2 GBq/µA) for 54 mm/ 1.7 GeV, with peak power-normalized yield at 150 MeV.

Single-shot ultrafast tomographic imaging by spectral multiplexing.

Computed tomography has profoundly impacted science, medicine and technology by using projection measurements scanned over multiple angles to permit cross-sectional imaging of an object. The application of computed tomography to moving or dynamically varying objects, however, has been limited by the temporal resolution of the technique, which is set by the time required to complete the scan. For objects that vary on ultrafast timescales, traditional scanning methods are not an option. Here we present a non-scanning method capable of resolving structure on femtosecond timescales by using spectral multiplexing of a single laser beam to perform tomographic imaging over a continuous range of angles simultaneously. We use this technique to demonstrate the first single-shot ultrafast computed tomography reconstructions and obtain previously inaccessible structure and position information for laser-induced plasma filaments. This development enables real-time tomographic imaging for ultrafast science, and offers a potential solution to the challenging problem of imaging through scattering surfaces.

Low-emittance electron bunches from a laser-plasma accelerator measured using single-shot x-ray spectroscopy.

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.

Long-range persistence of femtosecond modulations on laser-plasma-accelerated electron beams.

Laser plasma accelerators have produced femtosecond electron bunches with a relative energy spread ranging from 100% to a few percent. Simulations indicate that the measured energy spread can be dominated by a correlated spread, with the slice spread significantly lower. Measurements of coherent optical transition radiation are presented for broad-energy-spread beams with laser-induced density and momentum modulations. The long-range (meter-scale) observation of coherent optical transition radiation indicates that the slice energy spread is below the percent level to preserve the modulations.

Spectral sidebands on a narrow-bandwidth optical probe as a broad-bandwidth THz pulse diagnostic.

Broad-bandwidth THz-domain electro-magnetic pulses are typically diagnosed through temporal electro-optic (EO) cross-correlation with an optical probe pulse. Single-shot time-domain measurements of the THz waveform involve complex setups at a bandwidth coverage limited by the probe bandwidth. Here we present an EO-based diagnostic directly in the spectral domain, relying on THz-induced optical sidebands on a narrow-bandwidth optical probe. Experiments are conducted with a 0.11-THz-bandwidth optical probe and a broadband source (0-8 THz detection bandwidth) rich in spectral features. The validity of the sideband diagnostic concept, its spectral resolution, sideband amplitude, and the effects of probe timing are studied. For probe pulses longer than the THz pulse, the sideband technique proves an accurate single-shot spectral diagnostic, with advantages in setup simplicity and bandwidth coverage no longer limited by the laser bandwidth.

Spectroscopy of betatron radiation emitted from laser-produced wakefield accelerated electrons.

X-ray betatron radiation is produced by oscillations of electrons in the intense focusing field of a laser-plasma accelerator. These hard x-rays show promise for use in femtosecond-scale time-resolved radiography of ultrafast processes. However, the spectral characteristics of betatron radiation have only been inferred from filter pack measurements. In order to achieve higher resolution spectral information about the betatron emission, we used an x-ray charge-coupled device to record the spectrum of betatron radiation, with a full width at half maximum resolution of 225 eV. In addition, we have recorded simultaneous electron and x-ray spectra along with x-ray images that allow for a determination of the betatron emission source size, as well as differences in the x-ray spectra as a function of the energy spectrum of accelerated electrons.

Formation of optical bullets in laser-driven plasma bubble accelerators.

Electron density bubbles--wake structures generated in plasma of density n(e) approximately 10(19) cm(-3) by the light pressure of intense ultrashort laser pulses--are shown to reshape weak copropagating probe pulses into optical "bullets." The bullets are reconstructed using frequency-domain interferometric techniques in order to visualize bubble formation. Bullets are confined in three dimensions to plasma-wavelength size, and exhibit higher intensity, broader spectrum and flatter temporal phase than surrounding probe light, evidence of their compression by the bubble. Bullets observed at 0.8 approximately < n(e) approximately < 1.2x10(19) cm(-3) provide the first observation of bubble formation below the electron capture threshold. At higher n(e), bullets appear with high shot-to-shot stability together with relativistic electrons that vary widely in spectrum, and help relate bubble formation to fast electron generation.

Wavefront-sensor-based electron density measurements for laser-plasma accelerators.

Characterization of the electron density in laser produced plasmas is presented using direct wavefront analysis of a probe laser beam. The performance of a laser-driven plasma-wakefield accelerator depends on the plasma wavelength and hence on the electron density. Density measurements using a conventional folded-wave interferometer and using a commercial wavefront sensor are compared for different regimes of the laser-plasma accelerator. It is shown that direct wavefront measurements agree with interferometric measurements and, because of the robustness of the compact commercial device, offer greater phase sensitivity and straightforward analysis, improving shot-to-shot plasma density diagnostics.

Single-shot measurement of the spectral envelope of broad-bandwidth terahertz pulses from femtosecond electron bunches.

We present a new approach (demonstrated experimentally and through modeling) to characterize the spectral envelope of a terahertz (THz) pulse in a single shot. The coherent THz pulse is produced by a femtosecond electron bunch and contains information on the bunch duration. The technique, involving a single low-power laser probe pulse, is an extension of the conventional spectral encoding method (limited in time resolution to hundreds of femtoseconds) into a regime only limited in resolution by the laser pulse length (tens of femtoseconds). While only the bunch duration is retrieved (and not the exact charge profile), such a measurement provides a useful and critical parameter for optimization of the electron accelerator.

Single-beam and enhanced two-beam second-harmonic generation from silicon nanocrystals by use of spatially inhomogeneous femtosecond pulses.

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.

Single-shot measurement of temporal phase shifts by frequency-domain holography.

Frequency-domain holography is used to measure ultrafast phase shifts induced either by the nonlinear susceptibility ?(3) of fused silica or by ionization fronts in air over a temporal region of 1 ps with 70-fs resolution in a single shot. The use of an imaging spectrometer adds one-dimensional spatial resolution to the single-shot temporal measurements.