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.

One-joule 500-Hz cryogenic Yb:YAG laser driver of composite thin-disk design.

We present results on the development of a cryogenic Yb:YAG multi-pass laser amplifier based on a composite thin-disk design and demonstrate one-joule, diffraction limited, chirped 234-ps pulses with 50% optical-to-optical efficiency. High beam quality was obtained for repetition rates up to 400 Hz. The hardware was disassembled and thoroughly inspected after accumulating 80 hours of use at repetition rates from 100 to 500 Hz and exhibited no signs of damage. This laser driver is now commissioned to a dedicated laboratory where a grating compressor is producing 5.2-ps pulses used in the development of a compact x ray source based on inverse Compton scattering.

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.

Polarization-state-resolved high-harmonic spectroscopy of solids.

Attosecond metrology sensitive to sub-optical-cycle electronic and structural dynamics is opening up new avenues for ultrafast spectroscopy of condensed matter. Using intense lightwaves to precisely control the fast carrier dynamics in crystals holds great promise for next-generation petahertz electronics and devices. The carrier dynamics can produce high-order harmonics of the driving field extending up into the extreme-ultraviolet region. Here, we introduce polarization-state-resolved high-harmonic spectroscopy of solids, which provides deeper insights into both electronic and structural sub-cycle dynamics. Performing high-harmonic generation measurements from silicon and quartz, we demonstrate that the polarization states of the harmonics are not only determined by crystal symmetries, but can be dynamically controlled, as a consequence of the intertwined interband and intraband electronic dynamics. We exploit this symmetry-dynamics duality to efficiently generate coherent circularly polarized harmonics from elliptically polarized pulses. Our experimental results are supported by ab-initio simulations, providing evidence for the microscopic origin of the phenomenon.

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.

Pre-chirp managed, core-pumped nonlinear PM fiber amplifier delivering sub-100-fs and high energy (10 nJ) pulses with low noise.

We demonstrate a pre-chirp managed amplification (PCMA) system that is based on two stages of core-pumped, polarization maintaining (PM) fiber amplifiers. It produces output pulses with <65 fs duration and >10 nJ pulse energy from single-mode fibers. Tailoring of the spectra in the amplification chain enables pulse compression to near-perfect transform limited pulses (Strehl-ratio >0.9) and low intensity noise levels (0.008%) despite B-integrals >40 rad in the PCMA amplifier. Design strategies are presented. We expect this PCMA system to become an easy to implement add-on to a variety of existing sources while maintaining the advantages of the robustness of the PM standard fiber format.

250 W average power, 100 kHz repetition rate cryogenic Yb:YAG amplifier for OPCPA pumping.

A cryogenically cooled, bulk Yb:YAG, four-pass amplifier delivering up to 250 W average power at 100 kHz repetition rate is reported. The 2.5 mJ amplified optical pulses show a sub-20 ps duration before temporal compression and a spectrum supporting a transform-limited duration of 3.6 ps. The power instabilities were measured to be <0.5% rms over 30 min at full power, and the spatial intensity profile showed a flat-top distribution and near diffraction-limited beam quality. This compact amplifier is an ideal source for pumping either near-IR or mid-IR optical parametric chirped pulse amplifiers.

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.

All fiber-coupled, long-term stable timing distribution for free-electron lasers with few-femtosecond jitter.

We report recent progress made in a complete fiber-optic, high-precision, long-term stable timing distribution system for synchronization of next generation X-ray free-electron lasers. Timing jitter characterization of the master laser shows less than 170-as RMS integrated jitter for frequencies above 10 kHz, limited by the detection noise floor. Timing stabilization of a 3.5-km polarization-maintaining fiber link is successfully achieved with an RMS drift of 3.3 fs over 200 h of operation using all fiber-coupled elements. This all fiber-optic implementation will greatly reduce the complexity of optical alignment in timing distribution systems and improve the overall mechanical and timing stability of the system.

High-density Au nanorod optical field-emitter arrays.

We demonstrate the design, fabrication, characterization, and operation of high-density arrays of Au nanorod electron emitters, fabricated by high-resolution electron beam lithography, and excited by ultrafast femtosecond near-infrared radiation. Electron emission characteristic of multiphoton absorption has been observed at low laser fluence, as indicated by the power-law scaling of emission current with applied optical power. The onset of space-charge-limited current and strong optical field emission has been investigated so as to determine the mechanism of electron emission at high incident laser fluence. Laser-induced structural damage has been observed at applied optical fields above 5 GV m(-1), and energy spectra of emitted electrons have been measured using an electron time-of-flight spectrometer.

Remote two-color optical-to-optical synchronization between two passively mode-locked lasers.

Using balanced detection in both the radio frequency (RF) and the optical domain, we remotely synchronize the repetition rate of a Ti:sapphire oscillator to an Er-doped fiber oscillator through a 360 m length-stabilized dispersion compensated fiber link. The drift between these two optical oscillators is 3.3 fs root mean square (rms) over 24 hours. The 68 MHz Er-doped fiber oscillator is locked to a 476 MHz local RF reference clock, and serves as a master clock to distribute 10 fs-level timing signals through stabilized fiber links. This steady remote two-color optical-to-optical synchronization is an important step toward an integrated femtosecond fiber timing distribution system for free-electron lasers (FELs); it does not require x-ray pulses, and it makes sub-10-fs optical/x-ray pump-probe experiments feasible.

Pulse synthesis in the single-cycle regime from independent mode-locked lasers using attosecond-precision feedback.

We report the synthesis of a nearly single-cycle (3.7 fs), ultrafast optical pulse train at 78 MHz from the coherent combination of a passively mode-locked Ti:sapphire laser (6 fs pulses) and a fiber supercontinuum (1-1.4 µm, with 8 fs pulses). The coherent combination is achieved via orthogonal, attosecond-precision synchronization of both pulse envelope timing and carrier envelope phase using balanced optical cross-correlation and balanced homodyne detection, respectively. The resulting pulse envelope, which is only 1.1 optical cycles in duration, is retrieved with two-dimensional spectral shearing interferometry (2DSI). To our knowledge, this work represents the first stable synthesis of few-cycle pulses from independent laser sources.

Intense superradiant x rays from a compact source using a nanocathode array and emittance exchange.

A novel method of producing intense short wavelength radiation from relativistic electrons is described. The electrons are periodically bunched at the wavelength of interest enabling in-phase superradiant emission that is far more intense than from unbunched electrons. The periodic bunching is achieved in steps beginning with an array of beamlets emitted from a nanoengineered field emission array. The beamlets are then manipulated and converted to a longitudinal density modulation via a transverse-to-longitudinal emittance exchange. Periodic bunching at short wavelength is shown to be possible, and the partially coherent x-ray properties produced by inverse Compton scattering from an intense laser are estimated. The proposed method increases the efficiency of x-ray production by several orders of magnitude, potentially enabling compact x-ray sources to produce brilliance and flux similar to major synchrotron facilities.

Coherent synthesis of ultra-broadband optical parametric amplifiers.

We report on coherent synthesis of two ultra-broadband optical parametric amplifiers, each compressed by chirped mirror pairs, resulting in almost-octave-spanning (520-1000 nm) spectra supporting nearly single-cycle sub-4 fs pulse duration. Synthesized pulse timing is locked to less than 30 as by a balanced optical cross-correlator. The synthesized pulse is characterized by two-dimensional spectral interferometry and has a 3.8 fs duration.

Dynamics of actively mode-locked Quantum Cascade Lasers.

The impact of upper state lifetime and spatial hole burning on pulse shape and stability in actively mode locked QCLs is investigated by numerical simulations. It is shown that an extended upper state lifetime is necessary to achieve stable isolated pulse formation per roundtrip. Spatial hole burning helps to reduce the pulse duration by supporting broadband multimode lasing, but introduces pulse instabilities which eventually lead to strongly structured pulse shapes that further degrade with increased pumping. At high pumping levels gain saturation and recovery between pulses leads to suppression of mode locking. In the absence of spatial hole burning the laser approaches single-mode lasing, while in the presence of spatial hole burning the mode locking becomes unstable and the laser dynamics does not reach a steady state anymore.

Sub-two-cycle pulses by soliton self-compression in highly nonlinear photonic crystal fibers.

We demonstrate the direct generation of sub-two-cycle pulses by soliton self-compression of femtosecond pulses from a Ti:sapphire laser at 85 MHz using a 4.85-mm-long highly nonlinear photonic crystal fiber. Sub-nanojoule, 41 fs input pulses were compressed down to 4.6 fs without additional phase compensation schemes. To our knowledge, these are the shortest pulses obtained by soliton-effect compression of a laser oscillator. Efficient, near-dispersionless collimation of the fiber output was achieved with a simple lens and an octave-spanning double-chirped mirror pair. The full electric field of the compressed pulses was retrieved with a genetic algorithm applied to spectral and interferometric autocorrelation measurements, and the results are well described by numerical simulations.

Generation of <7 fs pulses at 800 nm from a blue-pumped optical parametric amplifier at degeneracy.

We generate ultrabroadband pulses at 800 nm from an optical parametric amplifier (OPA) pumped by the second harmonic of a Ti:sapphire system and working at degeneracy. The OPA is seeded by a white-light continuum generated from a near-IR OPA pumped by the same laser. Nearly transform-limited <7 fs pulses, fully characterized in amplitude and phase, are obtained with a chirped mirror compressor. The system fills the gap around 800 nm for broadband continuum seeded OPAs pumped by Ti:sapphire-based sources.