S. Sebban

Non-thermal melting in semiconductors measured at femtosecond resolution

Ultrafast time-resolved optical spectroscopy has revealed new classes of physical, chemical and biological reactions, in which directed, deterministic motions of atoms have a key role. This contrasts with the random, diffusive motion of atoms across activation barriers that typically determines kinetic rates on slower timescales. An example of these new processes is the ultrafast melting of semiconductors, which is believed to arise from a strong modification of the inter-atomic forces owing to laser-induced promotion of a large fraction (10% or more) of the valence electrons to the conduction band. The atoms immediately begin to move and rapidly gain sufficient kinetic energy to induce melting—much faster than the several picoseconds required to convert the electronic energy into thermal motions. Here we present measurements of the characteristic melting time of InSb with a recently developed technique of ultrafast time-resolved X-ray diffraction that, in contrast to optical spectroscopy, provides a direct probe of the changing atomic structure. The data establish unambiguously a loss of long-range order up to 900 Å inside the crystal, with time constants as short as 350 femtoseconds. This ability to obtain the quantitative structural characterization of non-thermal processes should find widespread application in the study of ultrafast dynamics in other physical, chemical and biological systems.

A high-intensity highly coherent soft X-ray femtosecond laser seeded by a high harmonic beam

Synchrotrons have for decades provided invaluable sources of soft X-rays, the application of which has led to significant progress in many areas of science and technology. But future applications of soft X-rays—in structural biology, for example—anticipate the need for pulses with much shorter duration (femtoseconds) and much higher energy (millijoules) than those delivered by synchrotrons. Soft X-ray free-electron lasers should fulfil these requirements but will be limited in number; the pressure on beamtime is therefore likely to be considerable. Laser-driven soft X-ray sources offer a comparatively inexpensive and widely available alternative, but have encountered practical bottlenecks in the quest for high intensities. Here we establish and characterize a soft X-ray laser chain that shows how these bottlenecks can in principle be overcome. By combining the high optical quality available from high-harmonic laser sources (as a seed beam) with a highly energetic soft X-ray laser plasma amplifier, we produce a tabletop soft X-ray femtosecond laser operating at 10 Hz and exhibiting full saturation, high energy, high coherence and full polarization. This technique should be readily applicable on all existing laser-driven soft X-ray facilities.

All-optical Compton gamma-ray source

Scientists demonstrate a Compton-based electromagnetic source based on a laser-plasma accelerator and a plasma mirror. The source generates a broadband spectrum of X-rays and is 10,000 times brighter than Compton X-ray sources based on conventional accelerators.

Single shot phase contrast imaging using laser-produced Betatron x-ray beams.

Development of x-ray phase contrast imaging applications with a laboratory scale source have been limited by the long exposure time needed to obtain one image. We demonstrate, using the Betatron x-ray radiation produced when electrons are accelerated and wiggled in the laser-wakefield cavity, that a high-quality phase contrast image of a complex object (here, a bee), located in air, can be obtained with a single laser shot. The Betatron x-ray source used in this proof of principle experiment has a source diameter of 1.7 μm and produces a synchrotron spectrum with critical energy E(c)=12.3±2.5 keV and 10⁹ photons per shot in the whole spectrum.

Polarization control of high order harmonics in the EUV photon energy range

We report the generation of circularly polarized high order harmonics in the extreme ultraviolet range (18-27 nm) from a linearly polarized infrared laser (40 fs, 0.25 TW) focused into a neon filled gas cell. To circularly polarize the initially linearly polarized harmonics we have implemented a four-reflector phase-shifter. Fully circularly polarized radiation has been obtained with an efficiency of a few percents, thus being significantly more efficient than currently demonstrated direct generation of elliptically polarized harmonics. This demonstration opens up new experimental capabilities based on high order harmonics, for example, in biology and materials science. The inherent femtosecond time resolution of high order harmonic generating table top laser sources renders these an ideal tool for the investigation of ultrafast magnetization dynamics now that the magnetic circular dichroism at the absorption M-edges of transition metals can be exploited.

Demonstration of the synchrotron-type spectrum of laser-produced Betatron radiation

Betatron x-ray radiation in laser–plasma accelerators is produced when electrons are accelerated and wiggled in the laser-wakefield cavity. This femtosecond source, producing intense x-ray beams in the multi-kiloelectronvolt (keV) range, has been observed at different interaction regimes using a high-power laser from 10 to 100 TW. However, none of the spectral measurements carried out were at sufficient resolution, bandwidth and signal-to-noise ratio to precisely determine the shape of spectra with a single laser shot in order to avoid shot-to-shot fluctuations. In this paper, the Betatron radiation produced using a 80 TW laser is characterized by using a single photon counting method. We measure in a single shot spectra from 8 to 21 keV with a resolution better than 350 eV. The results obtained are in excellent agreement with theoretical predictions and demonstrate the synchrotron-type nature of this radiation mechanism. The critical energy is found to be Ec=5.6±1 keV for our experimental conditions. In addition, the features of the source at this energy range open up novel opportunities for applications in time-resolved x-ray science.

Non-thermal desorption/ablation of molecular solids induced by ultra-short soft x-ray pulses

We report the first observation of single-shot soft x-ray laser induced desorption occurring below the ablation threshold in a thin layer of poly (methyl methacrylate)--PMMA. Irradiated by the focused beam from the Free-electron LASer in Hamburg (FLASH) at 21.7 nm, the samples have been investigated by atomic-force microscope (AFM) enabling the visualization of mild surface modifications caused by the desorption. A model describing non-thermal desorption and ablation has been developed and used to analyze single-shot imprints in PMMA. An intermediate regime of materials removal has been found, confirming model predictions. We also report below-threshold multiple-shot desorption of PMMA induced by high-order harmonics (HOH) at 32 nm. Short-time exposure imprints provide sufficient information about transverse beam profile in HOHs tight focus whereas long-time exposed PMMA exhibits radiation-initiated surface ardening making the beam profile measurement infeasible.

Towards enabling femtosecond helicity-dependent spectroscopy with high-harmonic sources

Recent advances in high-harmonic generation gave rise to soft X-ray pulses with higher intensity, shorter duration and higher photon energy. One of the remaining shortages of this source is its restriction to linear polarization, since the yield of generation of elliptically polarized high harmonics has been low so far. We here show how this limitation is overcome by using a cross-polarized two-colour laser field. With this simple technique, we reach high degrees of ellipticity (up to 75%) with efficiencies similar to classically generated linearly polarized harmonics. To demonstrate these features and to prove the capacity of our source for applications, we measure the X-ray magnetic circular dichroism (XMCD) effect of nickel at the M2,3 absorption edge around 67 eV. There results open up the way towards femtosecond time-resolved experiments using high harmonics exploiting the powerful element-sensitive XMCD effect and resolving the ultrafast magnetization dynamics of individual components in complex materials.

A proposal for multi-tens of GW fully coherent femtosecond soft X-ray lasers

X-ray free-electron lasers1, 2 delivering up to 1 × 1013 coherent photons in femtosecond pulses are bringing about a revolution in X-ray science3, 4, 5. However, some plasma-based soft X-ray lasers6 are attractive because they spontaneously emit an even higher number of photons (1 × 1015), but these are emitted in incoherent and long (hundreds of picoseconds) pulses7 as a consequence of the amplification of stochastic incoherent self-emission. Previous experimental attempts to seed such amplifiers with coherent femtosecond soft X-rays resulted in as yet unexplained weak amplification of the seed and strong amplification of incoherent spontaneous emission8. Using a time-dependent Maxwell–Bloch model describing the amplification of both coherent and incoherent soft X-rays in plasma, we explain the observed inefficiency and propose a new amplification scheme based on the seeding of stretched high harmonics using a transposition of chirped pulse amplification to soft X-rays. This scheme is able to deliver 5 × 1014 fully coherent soft X-ray photons in 200 fs pulses and with a peak power of 20 GW.

An optimized kHz two-colour high harmonic source for seeding free-electron lasers and plasma-based soft x-ray lasers

Free-electron lasers (FEL) and plasma-based soft x-ray lasers (PSXL) have been recently evolving very fast from the vacuum ultraviolet to the soft x-ray region. Once seeded with high harmonics, these schemes are considered as the next generation soft x-ray light sources delivering ultrashort pulses with high temporal and spatial coherence. Here, we present a detailed experimental study of a kHz two-colour high harmonic generation performed in various gases and investigate its potential as a suitable evolution of the actual seeding sources. It turns out that this double harmonic content source is highly tuneable, controllable and delivers intense radiation (measured here with a calibrated photodiode) with only one order of magnitude difference in the photon yield from 65 to 13?nm. Then, first and foremost, injections could be achieved at wavelengths shorter than what was previously accessible in FEL and PSXL and/or additional energy could be extracted. Also, such a strong and handy seed could allow the saturation range of FEL devices to be greatly extended to shorter wavelengths and would bring higher spectral as well as intensity stabilities in this spectral zone.