Laboratoire d'Optique Appliquée

In principle, the temporal beating of superposed high harmonics obtained by focusing a femtosecond laser pulse in a gas jet can produce a train of very short intensity spikes, depending on the relative phases of the harmonics. We present a method to measure such phases through two-photon, two-color photoionization. We found that the harmonics are locked in phase and form a train of 250-attosecond pulses in the time domain. Harmonic generation may be a promising source for attosecond time-resolved measurements.

The advent of ultraintense laser pulses generated by the technique of chirped pulse amplification (CPA) along with the development of high-fluence laser materials has opened up an entirely new field of optics. The electromagnetic field intensities produced by these techniques, in excess of ${10}^{18}\phantom{\rule{0.3em}{0ex}}\mathrm{W}∕{\mathrm{cm}}^{2}$, lead to relativistic electron motion in the laser field. The CPA method is reviewed and the future growth of laser technique is discussed, including the prospect of generating the ultimate power of a zettawatt. A number of consequences of relativistic-strength optical fields are surveyed. In contrast to the nonrelativistic regime, these laser fields are capable of moving matter more effectively, including motion in the direction of laser propagation. One of the consequences of this is wakefield generation, a relativistic version of optical rectification, in which longitudinal field effects could be as large as the transverse ones. In addition to this, other effects may occur, including relativistic focusing, relativistic transparency, nonlinear modulation and multiple harmonic generation, and strong coupling to matter and other fields (such as high-frequency radiation). A proper utilization of these phenomena and effects leads to the new technology of relativistic engineering, in which light-matter interactions in the relativistic regime drives the development of laser-driven accelerator science. A number of significant applications are reviewed, including the fast ignition of an inertially confined fusion target by short-pulsed laser energy and potential sources of energetic particles (electrons, protons, other ions, positrons, pions, etc.). The coupling of an intense laser field to matter also has implications for the study of the highest energies in astrophysics, such as ultrahigh-energy cosmic rays, with energies in excess of ${10}^{20}\phantom{\rule{0.3em}{0ex}}\mathrm{eV}$. The laser fields can be so intense as to make the accelerating field large enough for general relativistic effects (via the equivalence principle) to be examined in the laboratory. It will also enable one to access the nonlinear regime of quantum electrodynamics, where the effects of radiative damping are no longer negligible. Furthermore, when the fields are close to the Schwinger value, the vacuum can behave like a nonlinear medium in much the same way as ordinary dielectric matter expanded to laser radiation in the early days of laser research.

Although nonlinear methods can provide only the amplitude and the phase of an isolated ultrashort pulse, linear techniques can yield such measurements with a much better sensitivity and reliability when a reference pulse is available. We demonstrate two such methods, dual-quadrature spectral interferometry and Fourier-transform spectral interferometry. These techniques are simple to implement, very sensitive, and provide a complete measurement of the complex electric field, E(ω), as a continuous function of frequency.

Abstract This article gives an overall view of the mechanisms involved in the mesostructuring that takes place during the formation of surfactant‐templated inorganic materials by evaporation. Since such a method of preparation is well suited to fabricating thin films by dip coating, spin coating, casting, or spraying, it is of paramount interest to draw a general description of the processes occurring during the formation of self‐assembled hybrid organic/inorganic materials, taking into account all critical parameters. The following study is based on very recent works on the meso‐organization of thin silica films using tetraethylorthosilicate (TEOS) as the inorganic source and cetyltrimethylammonium bromide (CTAB) as the structuring agent, but we will show that the method can also be extended to other systems based on non‐silica oxides and block copolymer surfactants. We demonstrate that the organization depends mainly on the chemical composition of the film when it reaches the modulable steady state (MSS), where the inorganic framework is still flexible and the composition is stable after reaching an equilibrium in the diffusion of volatile species. This MSS state is generally attained seconds after the drying line, and the film's composition depends on various parameters: the relative vapor pressures in the environment, the evaporation conditions, and the chemical conditions in the initial solution. Diagrams of textures, in which the stabilized structures are controlled by local minima, are proposed to explain the complex phenomena associated with mesostructuring induced by evaporation.

Relativistic interaction of short-pulse lasers with underdense plasmas has recently led to the emergence of a novel generation of femtosecond x-ray sources. Based on radiation from electrons accelerated in plasma, these sources have the common properties to be compact and to deliver collimated, incoherent, and femtosecond radiation. In this article, within a unified formalism, the betatron radiation of trapped and accelerated electrons in the so-called bubble regime, the synchrotron radiation of laser-accelerated electrons in usual meter-scale undulators, the nonlinear Thomson scattering from relativistic electrons oscillating in an intense laser field, and the Thomson backscattered radiation of a laser beam by laser-accelerated electrons are reviewed. The underlying physics is presented using ideal models, the relevant parameters are defined, and analytical expressions providing the features of the sources are given. Numerical simulations and a summary of recent experimental results on the different mechanisms are also presented. Each section ends with the foreseen development of each scheme. Finally, one of the most promising applications of laser-plasma accelerators is discussed: the realization of a compact free-electron laser in the x-ray range of the spectrum. In the conclusion, the relevant parameters characterizing each sources are summarized. Considering typical laser-plasma interaction parameters obtained with currently available lasers, examples of the source features are given. The sources are then compared to each other in order to define their field of applications.

Fluorescence is widely used in optical devices, microscopy imaging, biology, medical research and diagnosis. Improving fluorescence sensitivity, all the way to the limit of single-molecular detection needed in many applications, remains a great challenge. The technique of surface enhanced fluorescence (SEF) is based upon the design of surfaces in the vicinity of the emitter. SEF yields an overall improvement in the fluorescence detection efficiency through modification and control of the local electromagnetic environment of the emitter. Near-field coupling between the emitter and surface modes plays a crucial role in SEF. In particular, plasmonic surfaces with localized and propagating surface plasmons are efficient SEF substrates. Recent progress in tailoring surfaces at the nanometre scale extends greatly the realm of SEF applications. This review focuses on the recent advances in the different mechanisms involved in SEF, in each case highlighting the most relevant applications.

We demonstrate that a beam of x-ray radiation can be generated by simply focusing a single high-intensity laser pulse into a gas jet. A millimeter-scale laser-produced plasma creates, accelerates, and wiggles an ultrashort and relativistic electron bunch. As they propagate in the ion channel produced in the wake of the laser pulse, the accelerated electrons undergo betatron oscillations, generating a femtosecond pulse of synchrotron radiation, which has keV energy and lies within a narrow (50 mrad) cone angle.

We study high-order harmonic generation in the general case of absorbing and dispersive atomic gas media. For ultrashort laser pulses, the harmonic conversion efficiency tends to a limit mainly imposed by the harmonic reabsorption in the gas. This limit, independent on the gas density, is the same for both the case of a loosely focused beam or a beam guided in a gas-filled hollow-core fiber. Under optimum conditions, we measured the highest conversion efficiency to date $(4\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}5})$ for the 15th harmonic generated in xenon using a 40 fs, 1.5 mJ, 800 nm pulse at a 1 kHz repetition rate.

The cholesteric-liquid-crystalline structure, which concerns the organization of chromatin, collagen, chitin, or cellulose, is omnipresent in living matter. In technology, it is found in temperature and pressure sensors, supertwisted nematic liquid crystal displays, optical filters, reflective devices, or cosmetics. A cholesteric liquid crystal reflects light because of its helical structure. The reflection is selective - the bandwidth is limited to a few tens of nanometers and the reflectance is equal to at most 50% for unpolarized incident light, which is a consequence of the polarization-selectivity rule. These limits must be exceeded for innovative applications like polarizer-free reflective displays, broadband polarizers, optical data storage media, polarization-independent devices, stealth technologies, or smart switchable reflective windows to control solar light and heat. Novel cholesteric-liquid-crystalline architectures with the related fabrication procedures must therefore be developed. This article reviews solutions found in living matter and laboratories to broaden the bandwidth around a central reflection wavelength, do without the polarization-selectivity rule and go beyond the reflectance limit.

Plasmas are an attractive medium for the next generation of particle accelerators because they can support electric fields greater than several hundred gigavolts per meter. These accelerating fields are generated by relativistic plasma waves-space-charge oscillations-that can be excited when a high-intensity laser propagates through a plasma. Large currents of background electrons can then be trapped and subsequently accelerated by these relativistic waves. In the forced laser wake field regime, where the laser pulse length is of the order of the plasma wavelength, we show that a gain in maximum electron energy of up to 200 megaelectronvolts can be achieved, along with an improvement in the quality of the ultrashort electron beam.

Biomedicine and cell and molecular biology require powerful imaging techniques of the single molecule scale to the whole organism, either for fundamental science or diagnosis. These applications are however often limited by the optical properties of the available probes. Moreover, in cell biology, the measurement of the cell response with spatial and temporal resolution is a central instrumental problem. This has been one of the main motivations for the development of new probes and imaging techniques either for biomolecule labeling or detection of an intracellular signaling species. The weak photostability of genetically encoded probes or organic dyes has motivated the interest for different types of nanoparticles for imaging such as quantum dots, nanodiamonds, dye-doped silica particles, or metallic nanoparticles. One of the most active fields of research in the past decade has thus been the development of rare-earth based nanoparticles, whose optical properties and low cytotoxicity are promising for biological applications. Attractive properties of rare-earth based nanoparticles include high photostability, absence of blinking, extremely narrow emission lines, large Stokes shifts, long lifetimes that can be exploited for retarded detection schemes, and facile functionalization strategies. The use of specific ions in their compositions can be moreover exploited for oxidant detection or for implementing potent contrast agents for magnetic resonance imaging. In this review, we present these different applications of rare-earth nanoparticles for biomolecule detection and imaging in vitro, in living cells or in small animals. We highlight how chemical composition tuning and surface functionalization lead to specific properties, which can be used for different imaging modalities. We discuss their performances for imaging in comparison with other probes and to what extent they could constitute a central tool in the future of molecular and cell biology.

The laminarity of high-current multi-MeV proton beams produced by irradiating thin metallic foils with ultraintense lasers has been measured. For proton energies $>10\text{ }\text{ }\mathrm{MeV}$, the transverse and longitudinal emittance are, respectively, $<0.004\text{ }\text{ }\mathrm{mm}\text{ }\mathrm{mrad}$ and $<{10}^{\ensuremath{-}4}\text{ }\text{ }\mathrm{eV}\text{ }\mathrm{s}$, i.e., at least 100-fold and may be as much as ${10}^{4}$-fold better than conventional accelerator beams. The fast acceleration being electrostatic from an initially cold surface, only collisions with the accelerating fast electrons appear to limit the beam laminarity. The ion beam source size is measured to be $<15\text{ }\ensuremath{\mu}\mathrm{m}$ (FWHM) for proton energies $>10\text{ }\text{ }\mathrm{MeV}$.

A very large high-energy shift of exciton resonances in GaAs multiple-quantum-well structures is observed during irradiation of the sample with femtosecond nonresonant radiation. This effect is discussed in terms of excitons "dressed" by photons.

We attribute a strong forward directed THz emission from femtosecond laser filaments in air to a transition-Cherenkov emission from the plasma space charge moving behind the ionization front at light velocity. Distant targets can be easily irradiated by this new source of THz radiation.

The localization and solvation of excess electrons in pure water have been resolved at the femtosecond time scale. Before it becomes solvated, the electron thermalizes and reaches in 110 fs a localized state absorbing in the infrared. This transient species with lifetime 240 fs has been postulated to exist but has not been observed previously in liquid water.

Conical emission in the forward direction is observed from intense femtosecond light pulses propagating through air over long distances. The conical emission is attributed to Cerenkov radiation from a dynamic self-guiding structure consisting of a weakly ionized core surrounded by Kerr cladding.

Bulk damage induced by fs IR laser pulses in silica is investigated both experimentally and numerically. In a strong focusing geometry, a first damage zone is followed by a narrow track with submicron width, indicating a filamentary propagation. The shape and size of the damage tracks are shown to correspond to the zone where the electron density created by optical field ionization and avalanche is close to ${10}^{20}\text{ }\text{ }{\mathrm{c}\mathrm{m}}^{\ensuremath{-}3}$. The relative role of avalanche and photoionization is studied. The plasma density produced in the wake of the pulse is shown to saturate around $2--4\ifmmode\times\else\texttimes\fi{}{10}^{20}\text{ }\text{ }{\mathrm{c}\mathrm{m}}^{\ensuremath{-}3}$.

We first obtain a frequency-space equation of diffraction tomography for the electric field vector, within the first-order Born approximation, using a simplified formalism resulting from using three-dimensional spatial frequencies and replacing outgoing waves by linear combinations of homogeneous plane waves. A coherent optical diffraction tomographic microscope is then described, in which a sample is successively illuminated by a series of plane waves having different directions, each scattered wave is recorded by phase-shifting interferometry, and the object is then reconstructed from these recorded waves. The measurement process in this device is analysed taking into account the illuminating wave, the wave scattered by the sample, the reference wave, and the phase relations between these waves. This analysis yields appropriate equations that take into account the characteristics of the reference wave and compensate random phase shifts. It makes it possible to obtain a high-resolution three-dimensional frequency representation in full conformity with theory. The experimentally obtained representations show index and absorptivity with a resolution limit of about a quarter of a wavelength, and have a depth of field of about 40 microm.

We take advantage of nonlinear properties associated with chi(3) tensor elements in BaF2 cubic crystal to improve the temporal contrast of femtosecond laser pulses. The technique presented is based on cross-polarized wave (XPW) generation. We have obtained a transmission efficiency of 10% and 10(-10) contrast with an input pulse in the millijoule range. This filter does not affect the spectral shape or the phase of the cleaned pulse. It also acts as an efficient spatial filter. In this method the contrast enhancement is limited only by the extinction ratio of the polarization discrimination device.