Sub-50 fs temporal resolution in an FEL-optical laser pump-probe experiment at FLASH2.

High temporal resolution is essential for ultra-fast pump-probe experiments. Arrival time jitter and drift measurements, as well as their control, become critical especially when combining XUV or X-ray free-electron lasers (FELs) with optical lasers due to the large scale of such facilities and their distinct pulse generation processes. This paper presents the application of a laser pulse arrival time monitor that actively corrects the arrival time of an optical laser relative to the FEL's main optical clock. Combined with post-analysis single pulse jitter correction this new approach improves the temporal resolution for pump-probe experiments significantly. Benchmark measurements on photo-ionization of xenon atoms performed at FLASH beamline FL26, demonstrate a sub-50 fs FWHM overall temporal resolution.

Parametric waveform synthesis: a scalable approach to generate sub-cycle optical transients.

The availability of electromagnetic pulses with controllable field waveform and extremely short duration, even below a single optical cycle, is imperative to fully harness strong-field processes and to gain insight into ultrafast light-driven mechanisms occurring in the attosecond time-domain. The recently demonstrated parametric waveform synthesis (PWS) introduces an energy-, power- and spectrum-scalable method to generate non-sinusoidal sub-cycle optical waveforms by coherently combining different phase-stable pulses attained via optical parametric amplifiers. Significant technological developments have been made to overcome the stability issues related to PWS and to obtain an effective and reliable waveform control system. Here we present the main ingredients enabling PWS technology. The design choices concerning the optical, mechanical and electronic setups are justified by analytical/numerical modeling and benchmarked by experimental observations. In its present incarnation, PWS technology enables the generation of field-controllable mJ-level few-femtosecond pulses spanning the visible to infrared range.

Strong-field coherent control of isolated attosecond pulse generation.

Attosecond science promises to reveal the most fundamental electronic dynamics occurring in matter and it can develop further by meeting two linked technological goals related to high-order harmonic sources: improved spectral tunability (allowing selectivity in addressing electronic transitions) and higher photon flux (permitting to measure low cross-section processes). New developments come through parametric waveform synthesis, which provides control over the shape of field transients, enabling the creation of highly-tunable isolated attosecond pulses via high-harmonic generation. Here we demonstrate that the first goal is fulfilled since central energy, spectral bandwidth/shape and temporal duration of isolated attosecond pulses can be controlled by shaping the laser waveform via two key parameters: the relative-phase between two halves of the multi-octave spanning spectrum, and the overall carrier-envelope phase. These results not only promise to expand the experimental possibilities in attosecond science, but also demonstrate coherent strong-field control of free-electron trajectories using tailored optical waveforms.

µJ-level multi-cycle terahertz generation in a periodically poled Rb:KTP crystal.

We demonstrate multi-cycle terahertz (MC-THz) generation in a 15.5 mm long periodically poled rubidium (Rb)-doped potassium titanyl phosphate (Rb:PPKTP) crystal with a poling period of 300 µm. By cryogenically cooling the crystal to 77 K, up to 0.72 µJ terahertz energy is obtained at a frequency of 0.5 THz with a 3 GHz bandwidth. A maximum internal optical-to-terahertz conversion efficiency of 0.16% is achieved, which is comparable with results achieved using periodically poled lithium niobate crystal. Neither photorefractive effects nor damage was observed with up to 900mJ/cm2, showing the great potential of Rb:PPKTP for multi-millijoule-level MC-THz generation.

Novel method for the angular chirp compensation of passively CEP-stable few-cycle pulses.

We demonstrate a novel, energy-efficient, cost-effective simple method for seeding CEP-stable OPCPAs. We couple the CEP-stable idler of a broadband OPCPA into a hollow core Kagome fiber thus compensating for the angular chirp. We obtain either relatively narrow bandwidths with ∼36% coupling efficiency or quarter-octave spanning bandwidths with ∼2.2% coupling efficiency. We demonstrate spectral compressibility, good beam quality and CEP stability. Our source is an ideal seed for high-energy, high-average power, CEP-stable few-cycle OPCPA pulses around 2 µm, which can drive the generation of coherent soft X-ray radiation in the water window spectral region via HHG.

CEP dependence of signal and idler upon pump-seed synchronization in optical parametric amplifiers.

We study the effect of pump-seed timing fluctuations on the carrier-envelope phase (CEP) of signal and idler pulses emerging from an OP(CP)A. A simple analytical model is derived in order to provide an intuitive explanation of the origin of CEP fluctuations, while split-step simulations are performed to cover a broad range of different seeding schemes. Finally, we compare the simulation results with real observations of the CEP of idler pulses generated by an OPA. The quantitative model presented provides a key tool for designing the next generation of low-noise CEP-stable OP(CP)A-based sources.

High-dynamic-range arrival time control for flexible, accurate and precise parametric sub-cycle waveform synthesis.

We introduce a simple all-inline variation of a balanced optical cross-correlator (BOC) that allows to measure the arrival time difference (ATD), over the full Nyquist bandwidth, with increased common-mode rejection and long-term stability. An FPGA-based signal processing unit allows for real-time signal normalization and enables locking to any setpoint with an unprecedented accuracy of 0.07 % within an increased ATD range of more than 400 fs, resulting in attosecond resolution locking. The setup precision is verified with an out-of-loop measurement to be less than 80 as residual jitter paving the way for highly demanding applications such as parametric waveform synthesizers.

40-µJ passively CEP-stable seed source for ytterbium-based high-energy optical waveform synthesizers.

We demonstrate experimentally for the first time a ~40-µJ two-octave-wide passively carrier-envelope phase (CEP)-stable parametric front-end for seeding an ytterbium (Yb)-pump-based, few-optical-cycle, high-energy optical parametric waveform synthesizer. The system includes a CEP-stable white-light continuum and two-channel optical parametric chirped pulse amplifiers (OPCPAs) in the near- and mid-infrared spectral regions spanning altogether a two-octave-wide spectrum driven by a regenerative amplifier. The output pulses are compressed and fully characterized to demonstrate the well-behaved spectral phase of this seed source.

Cascaded parametric amplification for highly efficient terahertz generation.

A highly efficient, practical approach to high-energy multi-cycle terahertz (THz) generation based on spectrally cascaded optical parametric amplification (THz-COPA) is introduced. Feasible designs are presented that enable the THz wave, initially generated by difference frequency generation between a narrowband optical pump and optical seed (0.1-10% of pump energy), to self-start a cascaded (or repeated) energy downconversion of pump photons in a single pass through a single crystal. In cryogenically cooled, periodically poled lithium niobate, unprecedented energy conversion efficiencies >8% achievable with existing pump laser technology are predicted using realistic simulations. The calculations account for cascading effects, absorption, dispersion, and laser-induced damage. Due to the simultaneous, coupled nonlinear evolution of multiple phase-matched three-wave mixing processes, THz-COPA exhibits physics distinctly different from conventional three-wave mixing parametric amplifiers. This, in turn, governs optimal phase-matching conditions, evolution of optical spectra, and limitations of the nonlinear process. Circumventing these limitations is shown to yield conversion efficiencies ≫10%.

Intracavity gain shaping in millijoule-level, high gain Ho:YLF regenerative amplifiers.

We demonstrate intracavity gain shaping inside a 2 µm Ho:YLF regenerative amplifier with a spectral bandwidth of 2.9 nm broadened to 5.4 nm, corresponding to Fourier-limited pulses of 1 ps duration. The intracavity gain shaping is achieved by using a simple etalon, which acts as a frequency-selective filter. The output of the regenerative amplifier is amplified by a single-pass amplifier, and we achieve total energy of 2.2 mJ and pulse duration of 2.4 ps at 1 kHz with pulse fluctuations <1%. The amplifier chain is seeded by a home-built mode-locked holmium-doped fiber oscillator.

White-light generation with sub-ps pulses.

We generate white light supercontinuum from slightly sub-picosecond pulses at 1.03 µm and 515 nm. We compare the spectra and stability for various crystals, focusing conditions and pulse durations, and determine the best parameters for sub-picosecond driver pulse duration. Comparing the experimental observations with the theory of white-light generation from Brodeur and Chin, it appears that in this particular range of pump pulse duration, two mechanisms interact and prevent a catastrophic collapse of the beam: multi-photon excitation (typical for ~100-fs-long pulses) and avalanche ionization (typical for >1-ps pulses). The two processes both manifest themselves in different experimental observations.

Terahertz generation in lithium niobate driven by Ti:sapphire laser pulses and its limitations.

We experimentally investigate the limits of 800-nm-to-terahertz (THz) energy conversion in lithium niobate at room temperature driven by amplified Ti:sapphire laser pulses with tilted pulse front. The influence of the pump central wavelength, pulse duration, and fluence on THz generation is studied. We achieved a high peak efficiency of 0.12% using transform limited 150 fs pulses and observed saturation of the optical-to-THz conversion efficiency at a fluence of 15 mJ/cm(2) for this pulse duration. We experimentally identify two main limitations for the scaling of optical-to-THz conversion efficiencies: (i) the large spectral broadening of the optical pump spectrum in combination with large angular dispersion of the tilted pulse front and (ii) free-carrier absorption of THz radiation due to multi-photon absorption of the 800 nm radiation.

Wavelength scaling of high harmonic generation close to the multiphoton ionization regime.

We study the wavelength scaling of high harmonic generation efficiency with visible driver wavelengths in the transition between the tunneling and the multiphoton ionization regimes where the Keldysh parameter is around unity. Our experiment shows a less dramatic wavelength scaling of efficiency than the conventional case for near- and mid-IR driver wavelengths, and it is well explained by a generalized three-step model for increased Keldysh parameters that employs complex ionization times in addition to the nonadiabatic ionization. The complex ionization time is critical to avoid the divergence when replacing the quasistatic ionization model by the more general nonadiabatic ionization model. Together, the two modifications present a consistent description of the influence of the atomic potential on the rescattering process in the intermediate Keldysh regime.

High-energy, phase-stable, ultrabroadband kHz OPCPA at 2.1 µm pumped by a picosecond cryogenic Yb:YAG laser.

We report on a kHz, mJ-level, carrier-envelope phase (CEP)-stable ultrabroadband optical parametric chirped-pulse amplifier (OPCPA) at 2.1-µm wavelength, pumped by a high-energy, 14 ps, cryogenic Yb:YAG pump laser, and its application to high-order harmonic generation (HHG) with Xe. The pre-amplifier chain is pumped by a 12-ps Nd:YLF pump laser and both pump lasers are optically synchronized to the signal pulse of the OPCPA. An amplified pulse energy of 0.85 mJ was obtained at the final OPCPA stage with good beam profile. The pulse is compressed to 4.5 optical cycles (<32 fs) with a spectral bandwidth of 474 nm supporting 3.5 optical cycles. The CEP stability was measured to be 194 mrad and the super-fluorescence noise is estimated to be ~9%. First HHG results are demonstrated with Xe showing significant cutoff extension to >85 eV with an efficiency of ~10-10 per harmonic, limited by the maximum gas pressure and flow into the chamber. This demonstrates the potential of this 2.1-µm source for scaling of photon energy and flux in the water-window range when applied to Ne and He at kHz repetition rate.

Observation and control of coherent torsional dynamics in a quinquethiophene molecule.

By applying femtosecond pump-probe spectroscopy to a substituted quinquethiophene molecule in solution, we observe in the time domain the coherent torsional dynamics that drives planarization of the excited state. Our interpretation is based on numerical modeling of the ground and excited state potential energy surfaces and simulation of wavepacket dynamics, which reveals two symmetric excited state deactivation pathways per oscillation period. We use the acquired knowledge on torsional dynamics to coherently control the excited state population with a pump-dump scheme, exploiting the non-stationary Franck-Condon overlap between ground and excited states.