HHG at the Carbon K-Edge Directly Driven by SRS Red-Shifted Pulses from an Ytterbium Amplifier.

In this work, we introduce a simplified approach to efficiently extend the high harmonic generation (HHG) cutoff in gases without the need for laser frequency conversion via parametric processes. Instead, we employ postcompression and red-shifting of a Yb:CaF2 laser via stimulated Raman scattering (SRS) in a nitrogen-filled stretched hollow core fiber. This driving scheme circumvents the low-efficiency window of parametric amplifiers in the 1100-1300 nm range. We demonstrate this approach being suitable for upscaling the power of a driver with an optimal wavelength for HHG in the highly desirable XUV range between 200 and 300 eV, up to the carbon K-edge. Due to the combination of power scalability of a low quantum defect ytterbium-based laser system with the high conversion efficiency of the SRS technique, we expect a significant increase in the generated photon flux in comparison with established platforms for HHG in the water window. We also compare HHG driven by the SRS scheme with the conventional self-phase modulation (SPM) scheme.

Capturing roaming molecular fragments in real time.

Since the discovery of roaming as an alternative molecular dissociation pathway in formaldehyde (H2CO), it has been indirectly observed in numerous molecules. The phenomenon describes a frustrated dissociation with fragments roaming at relatively large interatomic distances rather than following conventional transition-state dissociation; incipient radicals from the parent molecule self-react to form molecular products. Roaming has been identified spectroscopically through static product channel-resolved measurements, but not in real-time observations of the roaming fragment itself. Using time-resolved Coulomb explosion imaging (CEI), we directly imaged individual "roamers" on ultrafast time scales in the prototypical formaldehyde dissociation reaction. Using high-level first-principles simulations of all critical experimental steps, distinctive roaming signatures were identified. These were rendered observable by extracting rare stochastic events out of an overwhelming background using the highly sensitive CEI method.

Information transfer via temporal convolution in nonlinear optics.

Nonlinear parametric processes involving ultrashort pulses are typically carried out in time domain, which mathematically corresponds to a convolution of their frequency spectra. In contrast, this spectral convolution changes into a multiplication operation when performing the nonlinear interaction in frequency domain. Here, we extend the scope of frequency-domain nonlinear optics by demonstrating its ability to perform a temporal convolution. Through this approach, nonlinear optical operations that are inaccessible in time domain can be realised: specific optical information can be coherently advanced by picoseconds within a pulse sequence-a newly generated second harmonic pulse carries the amplitude and phase information of two input pulses. This central pulse is isolated when using an input field consisting of two cross-polarized input pulses in combination with type-II second harmonic generation. The effects of nonlinear temporal convolution can be viewed from the aspect of signal processing and pulse shaping, where the nonlinear interaction in the parametric crystal plays the role of a dynamic linear optical filter-in contrast to conventional static filters-with a shaping mask instantaneously adapting to the laser field.

Raman effect in the spectral broadening of ultrashort laser pulses in saturated versus unsaturated hydrocarbon molecules.

A conventional hollow core fiber (HCF) scheme is implemented to investigate spectral broadening of Titanium:Sapphire (Ti-Sa) femtosecond laser pulses in saturated hydrocarbon molecules compared to unsaturated ones. While the saturated molecules exhibit a spectral broadening similar to noble gases, for the unsaturated ones with π bonds, broadening towards blue is restrained. Numerical simulations underpin that it is a combination of group velocity dispersion (GVD) and Raman scattering which limits the spectral broadening for the unsaturated molecules. Compression of low energy ∼40fs pulses to ∼8fs using saturated hydrocarbons is demonstrated, suggesting the feasibility of this media for high repetition rate laser pulse compression.

Extremely broadband terahertz generation via pulse compression of an Ytterbium laser amplifier.

We present a system for extremely broadband terahertz (THz) generation based on an Ytterbium (Yb) amplified laser emitting 170-fs-long pulses centered at 1030 nm. The pulses are first spectrally broadened in an Ar-filled hollow-core capillary fiber (HCF) and then recompressed down to ∼18 fs with a chirped-mirror pair. Extreme broadband THz pulses of bandwidths up to 60 THz and peak electric field as high as 55 kV/cm are obtained via two-color plasma generation. The combination of high-power Yb laser systems with gas-filled HCF opens the path towards the realization of the next generation high-repetition-rate, extremely broadband, and intense-field THz time-domain spectroscopy systems.

Temporal characterization of femtosecond laser pulses using tunneling ionization in the UV, visible, and mid-IR ranges.

To generalize the applicability of the temporal characterization technique called "tunneling ionization with a perturbation for the time-domain observation of an electric field" (TIPTOE), the technique is examined in the multicycle regime over a broad wavelength range, from the UV to the IR range. The technique is rigorously analyzed first by solving the time-dependent Schrödinger equation. Then, experimental verification is demonstrated over an almost 5-octave wavelength range at 266, 1800, 4000 and 8000 nm by utilizing the same nonlinear medium - air. The experimentally obtained dispersion values of the materials used for the dispersion control show very good agreement with the ones calculated using the material dispersion data and the pulse duration results obtained for 1800 and 4000 nm agree well with the frequency-resolved optical gating measurements. The universality of TIPTOE arises from its phase-matching-free nature and its unprecedented broadband operation range.

Molecular gases for pulse compression in hollow core fibers.

We introduce hydrofluorocarbon molecules as an alternative medium to noble gases with low ionization potential like krypton or xenon to compress ultrashort pulses of relatively low energy in a conventional hollow core fiber with subsequent dispersion compensation. Spectral broadening of pulses from two different laser systems exceeded those achieved with argon and krypton. Initially 40 fs, 800 nm, 120 µJ pulses were compressed to few optical cycles duration. With the same approach a compression factor of more than 10 was demonstrated for an ytterbium-based laser (1030 nm, 170 fs, 200 µJ) leading to 15.6 fs.

Direct compression of 170-fs 50-cycle pulses down to 1.5 cycles with 70% transmission.

We present a straightforward route for extreme pulse compression, which relies on moderately driving self-phase modulation (SPM) over an extended propagation distance. This avoids that other detrimental nonlinear mechanisms take over and deteriorate the SPM process. The long propagation is obtained by means of a hollow-core fiber (HCF), up to 6 m in length. This concept is potentially scalable to TW pulse peak powers at kW average power level. As a proof of concept, we demonstrate 33-fold pulse compression of a 1 mJ, 6 kHz, 170 fs Yb laser down to 5.1 fs (1.5 cycles at 1030 nm), by employing a single HCF and subsequent chirped mirrors with an overall transmission of 70%.

Decoupling Frequencies, Amplitudes and Phases in Nonlinear Optics.

In linear optics, light fields do not mutually interact in a medium. However, they do mix when their field strength becomes comparable to electron binding energies in the so-called nonlinear optical regime. Such high fields are typically achieved with ultra-short laser pulses containing very broad frequency spectra where their amplitudes and phases are mutually coupled in a convolution process. Here, we describe a regime of nonlinear interactions without mixing of different frequencies. We demonstrate both in theory and experiment how frequency domain nonlinear optics overcomes the shortcomings arising from the convolution in conventional time domain interactions. We generate light fields with previously inaccessible properties by avoiding these uncontrolled couplings. Consequently, arbitrary phase functions are transferred linearly to other frequencies while preserving the general shape of the input spectrum. As a powerful application, we introduce deep UV phase control at 207 nm by using a conventional NIR pulse shaper.

Highly stable, 54mJ Yb-InnoSlab laser platform at 0.5kW average power.

We report on the leap of Yb-InnoSlab laser technology towards high pulse energies of 54mJ combined with high average power exceeding half a kW. The system features pulse durations of 1.5 picoseconds (ps) at 10kHz repetition rate with excellent beam properties (M2 of 1.1) combined with superb power and pointing stability in the sub-% range. It provides different output ports to facilitate optical synchronization for pumping parametric amplifiers. Tunable, femtosecond seed pulses are derived directly from the ps Yb pump pulses. We investigate the long term stability of this ps driven white light continuum and demonstrate 100-fold pulse compression down to 10fs duration. Ultra-broadband IR spectra centred at 2µm wavelength are subsequently generated via difference frequency generation of selected white light components.

Simple fiber-based solution for coherent multidimensional spectroscopy in the visible regime.

We report on a setup for coherent multidimensional spectroscopy based on visible continuum generation obtained by propagating 130 fs, <600 µJ pulses centered at 800 nm in a 2.5 m long hollow-core fiber. We find that with these modest input pulse requirements, the fiber can produce a stable, high brightness continuum spanning the 520-900 nm region, moreover in a single propagation step. The fiber exhibits 80% transmission, and the continuum features excellent spatial mode quality. In addition, spectral phase measurements suggest the possibility of a significantly self-compressed output in the visible, which simplifies aspects of the 2D spectrometer. The applicability of this simple, low-requirement source for 2D spectroscopy is demonstrated by performing a control experiment on the molecular dye Nile Blue.

Mid-infrared nonlinear absorption in As2S3 chalcogenide glass.

We report mid-infrared (MIR) nonlinear absorption in As2S3 glasses which results from two-photon excitation of valence electron to the Urbach extension followed by strong linear absorption of excited states. The measured MIR nonlinear absorption can be 3 to 4 orders of magnitude stronger than the two-photon absorption in the near-infrared for similar laser intensities and does not result from contaminants, but it is intrinsic to As2S3 glasses. As2S3 fibers are widely used to generate supercontinuum by pumping them with high peak power laser pulses. For a 100 kilowatt peak power MIR soliton propagating in single mode As2S3 fiber, the nonlinear absorption can be of similar magnitude than the fiber background loss. Finally, for laser peak power around 1 MW, the MIR nonlinear absorption can be ~2 orders of magnitude larger than the fiber background loss in single mode As2S3 fiber.

Multioctave infrared supercontinuum generation in large-core As2S3 fibers.

We report on infrared supercontinuum (SC) generation through laser filamentation and subsequent nonlinear propagation in a step-index As2S3 fiber. The 100 µm core and high-purity As2S3 fiber used exhibit zero-dispersion wavelength around 4.5 µm, a mid-infrared background loss of 0.2 dB/m, and a maximum loss of only 0.55 dB/m at the S-H absorption peak around 4.05 µm. When pumping with ultrashort laser pulses slightly above the S-H absorption band, broadband infrared supercontinua were generated with a 20 dB spectral flatness spanning from 1.5 up to 7 µm. The efficiency and spectral shape of the SC produced by ultrashort pulses in large-core As2S3 fiber are mainly determined by its dispersion, the S-H contaminant absorption, and the mid-infrared nonlinear absorption.

Tabletop imaging of structural evolutions in chemical reactions demonstrated for the acetylene cation.

The introduction of femto-chemistry has made it a primary goal to follow the nuclear and electronic evolution of a molecule in time and space as it undergoes a chemical reaction. Using Coulomb Explosion Imaging, we have shot the first high-resolution molecular movie of a to and fro isomerization process in the acetylene cation. So far, this kind of phenomenon could only be observed using vacuum ultraviolet light from a free-electron laser. Here we show that 266 nm ultrashort laser pulses are capable of initiating rich dynamics through multiphoton ionization. With our generally applicable tabletop approach that can be used for other small organic molecules, we have investigated two basic chemical reactions simultaneously: proton migration and C=C bond breaking, triggered by multiphoton ionization. The experimental results are in excellent agreement with the timescales and relaxation pathways predicted by new and quantitative ab initio trajectory simulations.

Frequency domain optical parametric amplification.

Today's ultrafast lasers operate at the physical limits of optical materials to reach extreme performances. Amplification of single-cycle laser pulses with their corresponding octave-spanning spectra still remains a formidable challenge since the universal dilemma of gain narrowing sets limits for both real level pumped amplifiers as well as parametric amplifiers. We demonstrate that employing parametric amplification in the frequency domain rather than in time domain opens up new design opportunities for ultrafast laser science, with the potential to generate single-cycle multi-terawatt pulses. Fundamental restrictions arising from phase mismatch and damage threshold of nonlinear laser crystals are not only circumvented but also exploited to produce a synergy between increased seed spectrum and increased pump energy. This concept was successfully demonstrated by generating carrier envelope phase stable, 1.43 mJ two-cycle pulses at 1.8 µm wavelength.

Mid-infrared supercontinuum generation in fluoroindate fiber.

We report the generation of mid-infrared supercontinua in a step-index fluoroindate-based fiber. The large core of the fluoroindate fiber allows the guiding of multiwatt laser power over a broad spectral range. These fibers exhibit zero dispersion at 1.83 µm, minimal loss of 0.1 dB/m at 3.2 µm up to only 0.8 dB/m at 5 µm. These specifications enable mid-infrared supercontinuum generation and propagation with low loss. By using mid-infrared ultrashort laser pulses from an optical parametric amplifier, we demonstrate generation of a 20 dB spectral flatness supercontinua from 2.7 to 4.7 µm in the fluoroindate fiber, which is twice the spectral broadening compared to a ZBLAN fiber under similar conditions.

Wavelength scaling of terahertz generation by gas ionization.

Low-frequency currents induced by ultrashort laser-driven ionization can emit extremely broadband, single-cycle terahertz pulses. We present a model that predicts a strong wavelength dependence of the THz emission in good agreement with our experimental study. This reveals that the combined effects of plasma currents rising proportionally to the square of the pump wavelength and wavelength-dependent focusing conditions lead to 30 times higher THz emission at 1800 nm compared to an 800 nm wavelength. Unrivaled single-cycle electric field strengths of 4.4 MV/cm are achieved with this compact table-top setup.

CEP stable 1.6 cycle laser pulses at 1.8 µm.

By using the novel approach for pulse compression that combines spectral broadening in hollow-core fiber (HCF) with linear propagation in fused silica (FS), we generate 1.6 cycle 0.24 mJ laser pulses at 1.8 µm wavelength with a repetition rate of 1 kHz. These pulses are obtained with a white light seeded optical parametric amplifier (OPA) and shown to be passively carrier envelope phase (CEP) stable.

Pulse compression of submillijoule few-optical-cycle infrared laser pulses using chirped mirrors.

We report generation of 400 microJ, 13.1 fs, 1425 nm optical parametric amplifier laser pulses. Spectral broadening of a 100 Hz optical parametric amplifier laser source is achieved by self-phase modulation in an argon-filled hollow-core fiber, and dispersion compensation is performed using chirped mirrors. This laser source will be useful for ultrafast time-resolved molecular orbital tomography.