Direct characterization of tuneable few-femtosecond dispersive-wave pulses in the deep UV.

Dispersive wave emission (DWE) in gas-filled hollow-core dielectric waveguides is a promising source of tuneable coherent and broadband radiation, but so far the generation of few-femtosecond pulses using this technique has not been demonstrated. Using in-vacuum frequency-resolved optical gating, we directly characterize tuneable 3 fs pulses in the deep ultraviolet generated via DWE. Through numerical simulations, we identify that the use of a pressure gradient in the waveguide is critical for the generation of short pulses.

Attosecond soft X-ray high harmonic generation.

High harmonic generation (HHG) of an intense laser pulse is a highly nonlinear optical phenomenon that provides the only proven source of tabletop attosecond pulses, and it is the key technology in attosecond science. Recent developments in high-intensity infrared lasers have extended HHG beyond its traditional domain of the XUV spectral range (10-150 eV) into the soft X-ray regime (150 eV to 3 keV), allowing the compactness, stability and sub-femtosecond duration of HHG to be combined with the atomic site specificity and electronic/structural sensitivity of X-ray spectroscopy. HHG in the soft X-ray spectral region has significant differences from HHG in the XUV, which necessitate new approaches to generating and characterizing attosecond pulses. Here, we examine the challenges and opportunities of soft X-ray HHG, and we use simulations to examine the optimal generating conditions for the development of high-flux, attosecond-duration pulses in the soft X-ray spectral range. This article is part of the theme issue 'Measurement of ultrafast electronic and structural dynamics with X-rays'.

Low-Energy Electron Emission in the Strong-Field Ionization of Rare Gas Clusters.

Clusters and nanoparticles have been widely investigated to determine how plasmonic near fields influence the strong-field induced energetic electron emission from finite systems. We focus on the contrary, i.e., the slow electrons, and discuss a hitherto unidentified low-energy structure (LES) in the photoemission spectra of rare gas clusters in intense near-infrared laser pulses. For Ar and Kr clusters we find, besides field-driven fast electrons, a robust and nearly isotropic emission of electrons with <4 eV kinetic energies that dominates the total yield. Molecular dynamics simulations reveal a correlated few-body decay process involving quasifree electrons and multiply excited ions in the nonequilibrium nanoplasma that results in a dominant LES feature. Our results indicate that the LES emission occurs after significant nanoplasma expansion, and that it is a generic phenomenon in intense laser nanoparticle interactions, which is likely to influence the formation of highly charged ions.

Spatio-temporal characterization of intense few-cycle 2 µm pulses.

We present a variant of spatially encoded spectral shearing interferometry for measuring two-dimensional spatio-temporal slices of few-cycle pulses centered around 2 µm. We demonstrate experimentally that the device accurately retrieves the pulse-front tilt caused by angular dispersion of two-cycle pulses. We then use the technique to characterize 500-650 µJ pulses from a hollow fiber pulse compressor, with durations as short as 7.1 fs (1.3 optical cycles).

Role of tunnel ionization in high harmonic generation from substituted benzenes.

We theoretically study high-harmonic generation in toluene, ortho-xylene and fluorobenzene driven by a 1.8 µm ultrashort pulse. We find that the chemical substitutions have a strong influence on the amplitude and phase of the emission from the highest occupied molecular orbital, despite having a small influence on the orbital itself. We show that this influence is due to the tunnel ionization step, which depends critically on the sign and amplitude of the asymptotic part of the wave function. We discuss how these effects would manifest in phase-sensitive high-harmonic generation spectroscopy experiments.

Three-wave mixing mediated femtosecond pulse compression in ß-barium borate.

Nonlinear pulse compression mediated by three-wave mixing is demonstrated for ultrashort Ti:sapphire pulses in a type II phase-matched ß-barium borate (BBO) crystal using noncollinear geometry. 170 µJ pulses at 800 nm with a pulse duration of 74 fs are compressed at their sum frequency to 32 fs with 55 µJ of pulse energy. Experiments and computer simulations demonstrate the potential of sum-frequency pulse compression to match the group velocities of the interacting waves to crystals that were initially not considered in the context of nonlinear pulse compression.

Generation of high-fidelity few-cycle pulses at 2.1 µm via cross-polarized wave generation.

We demonstrate the generation of temporally clean few-cycle pulses at 2.1 µm by shortening of 6-optical-cycle pulses via cross-polarized wave (XPW) generation in BaF(2), CaF(2) and CVD-Diamond crystals. By combining spectra and single-shot third-order intensity cross-correlation traces in a novel Bayesian pulse retrieval technique, we measured pulse durations of 20 fs, corresponding to 2.8 optical cycles. Our results show that XPW generation in the infrared could provide a high-fidelity source of few-cycle pulses for strong-field physics applications. It could also serve as an injector for high-peak power ultrafast mid-IR wavelength parametric amplifiers.

Three-dimensional spatiotemporal pulse characterization with an acousto-optic pulse shaper and a Hartmann-Shack wavefront sensor.

We demonstrate a simplified arrangement for spatiotemporal ultrashort pulse characterization called Hartmann-Shack assisted, multidimensional, shaper-based technique for electric-field reconstruction. It employs an acousto-optic pulse shaper in combination with a second-order nonlinear crystal and a Hartmann-Shack wavefront sensor. The shaper is used as a tunable bandpass filter, and the wavefronts and intensities of quasimonochromatic spectral slices of the pulse are obtained using the Hartmann-Shack wavefront sensor. The wavefronts and intensities of the spectral slices are related to one another using shaper-assisted frequency-resolved optical gating measurements, performed at particular points in the beam. This enables a three-dimensional reconstruction of the amplitude and phase of the pulse. We present some example pulse measurements and discuss the operating parameters of the device.

Few-cycle pulse characterization with an acousto-optic pulse shaper.

An acousto-optic pulse shaper has been used to characterize few-cycle pulses generated in a hollow-core fiber. A grism pair precompensates for the dispersion of the acousto-optic crystal, allowing the full pulse-shaping window to be used for replica generation rather than self-compensation. A 9.4 fs pulse was measured, the shortest ever measured with an acousto-optic pulse shaper, to our knowledge.

Lateral shearing interferometry of high-harmonic wavefronts.

We present a technique for frequency-resolved wavefront characterization of high harmonics based on lateral shearing interferometry. Tilted replicas of the driving laser pulse are produced by a Mach-Zehnder interferometer, producing separate focii in the target. The interference of the resulting harmonics on a flat-field extreme ultraviolet spectrometer yields the spatial phase derivative. A comprehensive set of spatial profiles, resolved by harmonic order, validate the technique and reveal the interplay of single-atom and macroscopic effects.

Extracting sub-cycle electronic and nuclear dynamics from high harmonic spectra.

We present a new methodology for measuring few-femtosecond electronic and nuclear dynamics in both atoms and polyatomic molecules using multidimensional high harmonic generation (HHG) spectroscopy measurements, in which the spectra are recorded as a function of the laser intensity to form a two-dimensional data set. The method is applied to xenon atoms and to benzene molecules, the latter exhibiting significant fast nuclear dynamics following ionization. We uncover the signature of the sub-cycle evolution of the returning electron flux in strong-field ionized xenon atoms, implicit in the strong field approximation but not previously observed directly. We furthermore extract the nuclear autocorrelation function in strong field ionized benzene cations, which is determined to have a decay of [Formula: see text] fs, in good agreement with the [Formula: see text] fs obtained from direct dynamics variational multi-configuration Gaussian calculations. Our method requires minimal assumptions about the system, and is applicable even to un-aligned polyatomic molecules.

Resolution of the relative phase ambiguity in spectral shearing interferometry of ultrashort pulses.

We show that multiple-shear spectral shearing interferometry can overcome the relative phase ambiguity of disjoint spectral components that is present in single-shear approaches. By upconverting the unknown pulse with spatially chirped ancillae, we achieve a shear-to-space mapping that can be acquired on an imaging spectrometer. A subset of this continuous range of shears can be chosen for robust and accurate phase retrieval using a multiple-shear algorithm.

Ultrashort pulse characterization by spectral shearing interferometry with spatially chirped ancillae.

We report a new version of spectral phase interferometry for direct electric field reconstruction (SPIDER), in which two spatially chirped ancilla fields are used to generate a spatially encoded SPIDER interferogram. We dub this new technique Spatially Encoded Arrangement for Chirped ARrangement for SPIDER (SEA-CAR-SPIDER). The single shot interferogram contains multiple shears, the spectral amplitude of the test pulse, and the reference phase, which is accurate for broadband pulses. The technique enables consistency checking through the simultaneous acquisition of multiple shears and offers a simple and precise calibration method. All calibration parameters--the shears, and the upconversionfrequency--can be accurately obtained from a single calibration trace.

Broadband astigmatism-free Czerny-Turner imaging spectrometer using spherical mirrors.

We describe the elimination of the astigmatism of a Czerny-Turner imaging spectrometer, built using spherical optics and a plane grating, over a broad spectral region. Starting with the principle of divergent illumination of the grating, which removes astigmatism at one chosen wavelength, we obtain design equations for the distance from the grating to the focusing mirror and the detector angle that remove the astigmatism to first order in wavelength. Experimentally, we demonstrate near diffraction-limited performance from 740 to 860 nm and over a 5 mm transverse spatial extent, while ray-tracing calculations show that barring finite-aperture and detector size limitations, this range extends from 640 to 900 nm and over 10 mm transversely. Our technique requires no additional optics and uses standard off-the-shelf components.

High-flux soft x-ray harmonic generation from ionization-shaped few-cycle laser pulses.

Laser-driven high-harmonic generation provides the only demonstrated route to generating stable, tabletop attosecond x-ray pulses but has low flux compared to other x-ray technologies. We show that high-harmonic generation can produce higher photon energies and flux by using higher laser intensities than are typical, strongly ionizing the medium and creating plasma that reshapes the driving laser field. We obtain high harmonics capable of supporting attosecond pulses up to photon energies of 600 eV and a photon flux inside the water window (284 to 540 eV) 10 times higher than previous attosecond sources. We demonstrate that operating in this regime is key for attosecond pulse generation in the x-ray range and will become increasingly important as harmonic generation moves to fields that drive even longer wavelengths.

Apparatus for soft x-ray table-top high harmonic generation.

There has been considerable recent interest in tabletop soft X-ray attosecond sources enabled by the new generation of intense, few-cycle laser sources at operating wavelengths longer than 800 nm. In our recent work [Johnson et al., Sci. Adv. 4(5), eaar3761 (2018)], we have demonstrated a new regime for the generation of X-ray attosecond pulses in the water window (284-540 eV) by high-harmonic generation, which resulted in soft X-ray fluxes of ≈109 photons/s and a maximum photon energy of 600 eV, an order of magnitude and 50 eV higher, respectively, than previously attained with few-cycle drivers. Here we present the key elements of our apparatus for the generation and detection of soft X-ray high harmonic radiation in the water window. Of critical importance is a differentially pumped gas target capable of supporting the multi-atmospheric pressures required to phase-match the high energy emission while strongly constraining the gas density, suppressing the effects of ionization and absorption outside the interaction region.

An apparatus for quantitative high-harmonic generation spectroscopy in molecular vapours.

We present an apparatus for performing gas phase high-harmonic generation spectroscopy of molecules primarily found in the liquid phase. Liquid molecular samples are heated in a temperature controlled bath and their vapour is used to back a continuous flow gas jet, with vapour pressures of over 1 bar possible. In order to demonstrate the system, we perform high harmonic spectroscopy experiments in benzene with a 1.8 µm driving field. Using the unique capabilities of the system, we obtain spectra that are nearly free from the effects of longitudinal phase-matching, amenable to comparison with advanced numerical modelling.

Dispersive wave blue-shift in supercontinuum generation.

We numerically study dispersive wave emission during femtosecond-pumped supercontinuum generation in photonic crystal fibres. We show that dispersive waves are primarily generated over a short region of high temporal compression. Despite the apparent complexity of the pump pulse in this region, we show that the dynamics of dispersive wave generation are dominated by a single fundamental soliton. However, any straightforward application of the theory that is thought to describe the blue emission, considerably underestimates the frequency shift. We show that in fact the red-shift of the soliton, caused by spectral recoil from the growing dispersive wave, causes an additional blue-shift of the resonant frequency which is in good agreement with full simulations.

Narrowband supercontinuum control using phase shaping.

We study theoretically, numerically and experimentally the effect of self-phase modulation of ultrashort pulses with spectrally narrow phase features. We show that spectral enhancement and depletion is caused by changing the relative phase between the initial field and the nonlinearly generated components. Our theoretical results explain observations of supercontinuum enhancement by fiber Bragg gratings, and predict similar enhancements for spectrally shaped pulses in uniform fiber. As proof of principle, we demonstrate this effect in the laboratory using a femtosecond pulse shaper.