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.

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.

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.

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 , Sci. Adv.

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.

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.

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.

Strong-field ionization of clusters using two-cycle pulses at 1.8 μm.

The interaction of intense laser pulses with nanoscale particles leads to the production of high-energy electrons, ions, neutral atoms, neutrons and photons. Up to now, investigations have focused on near-infrared to X-ray laser pulses consisting of many optical cycles. Here we study strong-field ionization of rare-gas clusters (10 to 10 atoms) using two-cycle 1.

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.

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.

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

Nonlinear pulse compression mediated by three-wave mixing is demonstrated for ultrashort Ti:sapphire pulses in a type II phase-matched β-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.

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.

Spatio-temporal focusing of an ultrafast pulse through a multiply scattering medium.

Pulses of light propagating through multiply scattering media undergo complex spatial and temporal distortions to form the familiar speckle pattern. There is much current interest in both the fundamental properties of speckles and the challenge of spatially and temporally refocusing behind scattering media. Here we report on the spatially and temporally resolved measurement of a speckle field produced by the propagation of an ultrafast optical pulse through a thick strongly scattering medium.

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.

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.

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.

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.

Improved ancilla preparation in spectral shearing interferometry for accurate ultrafast pulse characterization.

We report a version of spectral phase interferometry for direct electric field reconstruction (SPIDER), in which spectral filters are used to produce the quasi-monochromatic fields required for upconversion. The advantages of this approach include improved calibration accuracy, robustness for strongly chirped input pulses, simplicity, and compactness. We verify the technique experimentally by measuring the spectral chirp of a grating compressor using a spatially encoded arrangement (SEA-)SPIDER.

Tunable spectral enhancement of fiber supercontinuum.

We demonstrate tunable spectral enhancement of the supercontinuum generated in a microstructured fiber with a fiber long-period grating. The long-period grating leads to phase distortion and loss that, with subsequent high-intensity propagation in uniform fiber, evolves into an enhancement around the grating's resonant wavelengths. Wavelength tunability is achieved by varying the temperature or the ambient refractive index, and the spectral peak can be extinguished by immersing the grating in index-matching oil.

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.

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.