Phase-matching-free ultrashort laser pulse characterization from a transient plasma lens.

A phase-matching-free ultrashort pulse retrieval based on the defocusing of a laser-induced plasma is presented. In this technique, a pump pulse ionizes a rare gas providing a plasma lens whose creation time is ultrafast. A probe pulse propagating through this gas lens experiences a switch of its divergence. The spectrum of the diverging part, isolated by a coronograph, is measured as a function of the pump-probe delay, providing a spectrogram that allows for a comprehensive characterization of the temporal properties of the probe pulse. The method, called PI-FROSt for "plasma-induced frequency-resolved optical switching," is simple, is free of phase-matching constraints, and can operate in both self- and cross-referenced configurations at ultrahigh repetition rate in the whole transparency range of the gas. The assessment of the method demonstrates laser pulse reconstructions of high reliability in both near-infrared (NIR) and ultraviolet (UV) spectral ranges.

High-order parametric generation of coherent XUV radiation.

Extreme ultraviolet (XUV) radiation finds numerous applications in spectroscopy. When the XUV light is generated via high-order harmonic generation (HHG), it may be produced in the form of attosecond pulses, allowing access to unprecedented ultrafast phenomena. However, the HHG efficiency remains limited. Here we present an observation of a new regime of coherent XUV emission which has a potential to provide higher XUV intensity, vital for applications. We explain the process by high-order parametric generation, involving the combined emission of THz and XUV photons, where the phase matching is very robust against ionization. This introduces a way to use higher-energy driving pulses, thus generating more XUV photons.

Doppler effect as a tool for ultrashort electric field reconstruction.

We present a new, to the best of our knowledge, variant of the spectral-shearing interferometry method for characterizing ultrashort laser pulses. This original approach, called Doppler effect e-field replication (DEER), exploits the rotational Doppler effect for producing frequency shear and provides spectral shearing in the absence of frequency conversion, enabling operation in the ultraviolet spectral range. Evaluation of the DEER-spectral phase interferometry for direct electric field reconstruction setup reveals a phase reconstruction of great reliability. Possible improvements, benefits, and worthwhile prospects of the method are discussed.

BOAR: Biprism based optical autocorrelation with retrieval.

A simple and compact single-shot autocorrelator is presented and analyzed in detail. The autocorrelator is composed of two elements only: a Fresnel biprism used to create two temporally delayed replicas of the pulse to characterize and a camera in which two-photon absorption takes place. The two-photon absorption signal obtained in the camera can be used to retrieve the pulse duration, the frequency chirp, and the pulse spectrum, provided that a Gaussian temporal shape is assumed. Thanks to its extreme simplicity, the autocorrelator is robust and easy to align. The presented design can theoretically characterize the pulse duration from about 25 fs to 1.5 ps in the two-photon spectral range of the camera (1200-2400 nm). Finally, a proof-of-principle demonstration is also performed at 3.1 µm by using an InGaAs camera, whose two-photon spectral range is located further in the infrared (1800-3400 nm).

Optics-less focusing of XUV high-order harmonics.

By experimentally studying high-order harmonic beams generated in gases, we show how the spatial characteristics of these ultrashort extreme-ultraviolet (XUV) beams can be finely controlled when a single fundamental beam generates harmonics in a thin gas medium. We demonstrate that these XUV beams can be emitted as converging beams and thereby get focused after generation. We study this optics-less focusing using a spatially chirped beam that acts as a probe located inside the harmonic generation medium. We analyze the XUV beam evolution with an analytical model and obtain very good agreement with experimental measurements. The XUV foci sizes and positions vary strongly with the harmonic order, and the XUV waist can be located at arbitrarily large distances from the generating medium. We discuss how intense XUV fields can be obtained with optics-less focusing and how the order-dependent XUV beam characteristics are compatible with broadband XUV irradiation and attosecond science.

Time-Resolved Measurement of Interatomic Coulombic Decay Induced by Two-Photon Double Excitation of Ne_{2}.

The hitherto unexplored two-photon doubly excited states [Ne^{*}(2p^{-1}3s)]_{2} were experimentally identified using the seeded, fully coherent, intense extreme ultraviolet free-electron laser FERMI. These states undergo ultrafast interatomic Coulombic decay (ICD), which predominantly produces singly ionized dimers. In order to obtain the rate of ICD, the resulting yield of Ne_{2}^{+} ions was recorded as a function of delay between the extreme ultraviolet pump and UV probe laser pulses. The extracted lifetimes of the long-lived doubly excited states, 390(-130/+450) fs, and of the short-lived ones, less than 150 fs, are in good agreement with ab initio quantum mechanical calculations.

Slow Interatomic Coulombic Decay of Multiply Excited Neon Clusters.

Ne clusters (∼5000 atoms) were resonantly excited (2p→3s) by intense free electron laser (FEL) radiation at FERMI. Such multiply excited clusters can decay nonradiatively via energy exchange between at least two neighboring excited atoms. Benefiting from the precise tunability and narrow bandwidth of seeded FEL radiation, specific sites of the Ne clusters were probed. We found that the relaxation of cluster surface atoms proceeds via a sequence of interatomic or intermolecular Coulombic decay (ICD) processes while ICD of bulk atoms is additionally affected by the surrounding excited medium via inelastic electron scattering. For both cases, cluster excitations relax to atomic states prior to ICD, showing that this kind of ICD is rather slow (picosecond range). Controlling the average number of excitations per cluster via the FEL intensity allows a coarse tuning of the ICD rate.

Spatio-spectral structures in high-order harmonic beams generated with Terawatt 10-fs pulses.

A large international effort is nowadays devoted to increase the energy of the extreme ultraviolet pulses by using high-peak power ultrashort fundamental pulses (Terawatt level). Using such fundamental pulses brings specific constraints that need to be addressed. Here we study high-order harmonic generation in gases with 10 fs pulses at Terawatt peak power and demonstrate that extreme ultraviolet beams can be highly structured and complex in various conditions. We use a single-shot spatially resolved spectral detection and demonstrate direct observation of the spatio-temporal coupling occurring in the generating medium. Clear and reproducible complex spatio-spectral structures are observed in the far field. Similar structures are reproduced with simulations and we show that they are intimately associated to the high nonlinearity of high-order harmonic generation. Those findings are of prime importance for the generation of high-energy attosecond pulses and reveal important issues for their applications.

High-order harmonic generation from a dual-gas, multi-jet array with individual gas jet control.

We present a gas jet array for use in high-order harmonic generation experiments. Precise control of the pressure in each individual gas jet has allowed a thorough investigation into mechanisms contributing to the selective enhancement observed in the harmonic spectra produced by dual-gas, multi-jet arrays. Our results reveal that in our case, the dominant enhancement mechanism is the result of a compression of the harmonic-producing gas jet due to the presence of other gas jets in the array. The individual control of the gas jets in the array also provides a promising method for enhancing the harmonic yield by precise tailoring of the length and pressure gradient of the interaction region.

Conical intersection dynamics in NO2 probed by homodyne high-harmonic spectroscopy.

Conical intersections play a crucial role in the chemistry of most polyatomic molecules, ranging from the simplest bimolecular reactions to the photostability of DNA. The real-time study of the associated electronic dynamics poses a major challenge to the latest techniques of ultrafast measurement. We show that high-harmonic spectroscopy reveals oscillations in the electronic character that occur in nitrogen dioxide when a photoexcited wave packet crosses a conical intersection. At longer delays, we observe the onset of statistical dissociation dynamics. The present results demonstrate that high-harmonic spectroscopy could become a powerful tool to highlight electronic dynamics occurring along nonadiabatic chemical reaction pathways.

Phase characterization of the reflection on an extreme UV multilayer: comparison between attosecond metrology and standing wave measurements.

We characterize the phase shift induced by reflection on a multilayer mirror in the extreme UV range (80-93 eV) using two techniques: one based on high order harmonic generation and attosecond metrology (reconstruction of attosecond beating by interference of two-photon transitions), and a second based on synchrotron radiation and measurements of standing waves (total electron yield). We find an excellent agreement between the results from the two measurements and a flat group delay shift (±40 as) over the main reflectivity peak of the mirror.

Controlling high harmonics generation by spatial shaping of high-energy femtosecond beam.

We demonstrate controlled high-order harmonic generation in gas using high-energy femtosecond pulses (50 fs-50 mJ on target) by performing spatial shaping of the terrawatt fundamental laser beam. We have developed a two optical paths mirror that can withstand high power and shape the pump beam into a quasi-flat-top profile (super Gaussian) near focus. We observe clear signatures of the spatial shaping on the harmonic beam in terms of profile, divergence, level of signal, and spectrum. The harmonic generation in neon with a quasi-flat-top beam results in a broadband extreme UV beam with extremely low divergence (~340 µrad).

Post-compression of high-energy femtosecond pulses using gas ionization.

We present a new optical post-compression technique designed for high-energy ultrashort pulses. A large spectral broadening is achieved through rapid ionization of helium by an intense pulse (>10(15) W/cm(2)) propagating in a capillary filled with low-pressure helium. The blueshifted pulses are re-compressed with chirped mirrors and silica plates. From a terawatt Ti:sapphire laser chain providing pulses of 40 fs, 70 mJ, we demonstrate the compression of pulses down to 11.4 fs (FWHM) with a total output energy of 13.7 mJ.