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.

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.

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.

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.

Generation of broadband mid-infrared pulses from an optical parametric amplifier.

We report on the direct generation of broadband mid-IR pulses from an optical parametric amplifier. Several crystals with extended IR transparency, when pumped at 800 nm, display a broad phase-matching bandwidth around 1 mum, allowing for the generation of idler pulses spanning the 3-5 mum wavelength range. Using LiIO(3), we produce 2muJ pulses tunable in the 3-4 mum range with bandwidth supporting 30-fs transform-limited duration.

Narrow-bandwidth picosecond pulses by spectral compression of femtosecond pulses in second-order nonlinear crystals.

We introduce a simple approach for the efficient generation of tunable narrow-bandwidth picosecond pulses synchronized to broadband femtosecond ones. Second harmonic generation in the presence of large group velocity mismatch between the interacting pulses transfers a large fraction of the energy of a broadband fundamental frequency pulse into a narrowband second harmonic one. Using a periodically poled stoichiometric lithium tantalate crystal coupled to an infrared optical parametric amplifier, we generated 200-nJ pulses with spectral width lower than 8.5 cm(-1) and tunability from 720 to 890 nm. Energy scaling and extension of the tuning range are straightforward.

High-energy, few-optical-cycle pulses at 1.5 microm with passive carrier-envelope phase stabilization.

We report on a source of ultrabroadband self-phase-stabilized near-IR pulses by difference-frequency generation of a hollow-fiber broadened supercontinuum followed by two-stage optical parametric amplification. We demonstrate energies up to 200 microJ with 15 fs pulse width, making this source suited as a driver for attosecond pulse generation.

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.

Ultrafast manipulation of strong coupling in metal-molecular aggregate hybrid nanostructures.

We demonstrate an ultrafast manipulation of the Rabi splitting energy Ω(R) in a metal-molecular aggregate hybrid nanostructure. Femtosecond excitation drastically alters the optical properties of a model system formed by coating a gold nanoslit array with a thin J-aggregated dye layer. Controlled and reversible transient switching from strong (Ω(R) ≃ 55 meV) to weak (Ω(R) ≈ 0) coupling on a sub-ps time scale is directly evidenced by mapping the nonequilibrium dispersion relations of the coupled excitations. Such a strong, externally controllable coupling of excitons and surface plasmon polaritons is of considerable interest for ultrafast all-optical switching applications in nanoscale plasmonic circuits.

Sub-two-cycle light pulses at 1.6 microm from an optical parametric amplifier.

We generate ultrabroadband pulses, spanning the 1200-2100 nm wavelength range, from an 800 nm pumped optical parametric amplifier (OPA) working at degeneracy. We compress the microjoule-level energy pulses to nearly transform-limited 8.5 fs duration by an adaptive system employing a deformable mirror. To our knowledge, these are the shortest light pulses generated at 1.6 microm.

Few-optical-cycle pulses in the near-infrared from a noncollinear optical parametric amplifier.

We extend the concept of broadband phase matching in a noncollinear optical parametric amplifier (NOPA) to the near-IR. In an 800 nm pumped NOPA using periodically poled stoichiometric lithium tantalate, we amplify a spectrum spanning the 1.1-1.7 microm range and corresponding to two optical cycles of the carrier wavelength. A limited portion of the spectrum is compressed by a prism pair down to 16 fs.