H. Pépin

Tomographic imaging of molecular orbitals

Single-electron wavefunctions, or orbitals, are the mathematical constructs used to describe the multi-electron wavefunction of molecules. Because the highest-lying orbitals are responsible for chemical properties, they are of particular interest. To observe these orbitals change as bonds are formed and broken is to observe the essence of chemistry. Yet single orbitals are difficult to observe experimentally, and until now, this has been impossible on the timescale of chemical reactions. Here we demonstrate that the full three-dimensional structure of a single orbital can be imaged by a seemingly unlikely technique, using high harmonics generated from intense femtosecond laser pulses focused on aligned molecules. Applying this approach to a series of molecular alignments, we accomplish a tomographic reconstruction of the highest occupied molecular orbital of N2. The method also allows us to follow the attosecond dynamics of an electron wave packet.

Laser-Induced Electron Tunneling and Diffraction

Molecular structure is usually determined by measuring the diffraction pattern the molecule impresses on x-rays or electrons. We used a laser field to extract electrons from the molecule itself, accelerate them, and in some cases force them to recollide with and diffract from the parent ion, all within a fraction of a laser period. Here, we show that the momentum distribution of the extracted electron carries the fingerprint of the highest occupied molecular orbital, whereas the elastically scattered electrons reveal the position of the nuclear components of the molecule. Thus, in one comprehensive technology, the photoelectrons give detailed information about the electronic orbital and the position of the nuclei.

Filamentation of ultrashort pulse laser beams resulting from their propagation over long distances in air

The propagation of high-power short-pulse laser beams over considerable distances in air is studied both experimentally and via numerical simulations. Filaments are formed after 5–10 m and their propagation over distances in excess of 200 m is reported for the first time. The lateral dimensions of the filaments are found to range from about 100 μm to a few millimeters in diameter. The early values of plasma electron density have been inferred to be a few times 1016 cm−3 using longitudinal spectral interferometry. For 500 fs pulses and a wavelength of 1053 nm, the energy in the filament can be quite high initially (∼8 mJ) and is found to stabilize at about 1.5–2 mJ, after about 35 m. A simple model based on the nonlinear Schrodinger equation coupled to a multiphoton ionization law appears to describe several experimental results quite well.

Triggering and guiding high-voltage large-scale leader discharges with sub-joule ultrashort laser pulses*

The triggering and guiding of leader discharges using a plasma channel created by a sub-joule ultrashort laser pulse have been studied in a megavolt large-scale electrode configuration (3–7 m rod-plane air gap). By focusing the laser close to the positive rod electrode it has been possible, with a 400 mJ pulse, to trigger and guide leaders over distances of 3 m, to lower the leader inception voltage by 50%, and to increase the leader velocity by a factor of 10. The dynamics of the breakdown discharges with and without the laser pulse have been analyzed by means of a streak camera and of electric field and current probes. Numerical simulations have successfully reproduced many of the experimental results obtained with and without the presence of the laser plasma channel.

Ultrafast x‐ray sources*

Time‐resolved spectroscopy (with a 2 psec temporal resolution) of plasmas produced by the interaction between solid targets and a high contrast subpicosecond table top terawatt (T3) laser at 1016 W/cm2, is used to study the basic processes which control the x‐ray pulse duration. Short x‐ray pulses have been obtained by spectral selection or by plasma gradient scalelength control. Time‐dependent calculations of the atomic physics [Phys. Fluids B 4, 2007, 1992] coupled to a Fokker–Planck code [Phys. Rev. Lett. 53, 1461, 1984] indicate that it is essential to take into account the non‐Maxwellian character of the electron distribution for a quantitative analysis of the experimental results.

Effect of rapid thermal annealing on both the stress and the bonding states of a-SiC:H films

The stress evolution of plasma enhanced chemical vapor deposition a‐SiC:H films was studied by increasing the annealing temperature from 300 to 850 °C. A large stress range from −1 GPa compressive to 1 GPa tensile was investigated. Infrared absorption, x‐ray photoelectron spectroscopy, and elastic recoil detection analysis techniques were used to follow the Si‐C, Si‐H, and C‐H absorption band evolutions, the Si2p and C1s chemical bondings, and the a‐SiC:H film hydrogen content variations with the annealing temperatures, respectively. It is pointed out that the compressive stress relaxation is due to the hydrogenated bond (Si—H and C—H) dissociation, whereas the tensile stress is caused by additional Si—C bond formation. At high annealing temperatures, a total hydrogen content decrease is clearly observed. This total hydrogen loss is interpreted in terms of hydrogen molecule formation and outerdiffusion. The results are discussed and a quantitative model correlating the intrinsic stress variation to the Si...

A study of the effect of composition on the microstructural evolution of a–Si x C 1 − x : H PECVD films: IR absorption and XPS characterizations

Amorphous silicon carbide films (a–Si x C 1 − x :H) deposited by the argon- or helium-diluted PECVD technique were studied as a function of their composition. Microstructural investigations were mainly achieved by means of FTIR and XPS techniques. Nuclear techniques were used to obtain precise information on the film hydrogen content. The Si–H IR-absorption band was deconvoluted in different monohydride and dihydride silicon environments. The existence of SiH 2 bonds in the Si-rich composition was evidenced. From the analysis of the C–H and Si–H absorption bands it is shown that hydrogen atoms are preferentially bonded to carbon atoms. The deconvolution of the Si 2 p core level peak suggests that above a composition of x ∊ 0.5, the noncarburized (Si, Si, H) local environment contribution increases to the detriment of the hydrocarburized (Si, C, H) environments. From the evolution of the C 1 s peak, it can be deduced that there is a change in the carbon atom bonding states when the film composition is varied. These results are correlated and discussed in terms of the local bonding environments and their evolution with film composition.

Modeling the triggering of streamers in air by ultrashort laser pulses

The physical processes involved in the triggering of ionization waves (streamers) by ultrashort laser pulses, focused in air at 350 Torr and in a uniform electric field, are investigated by means of a one-dimensional (1-D) numerical model. The model describes the interaction of the laser pulse with air and takes into account many of the reactions in the laser-created plasma as well as the radial expansion of the plasma. Consequences of the model are that the threshold electric field for the appearance of streamers is an increasing function of the delay between the laser pulse and the electric field pulse and a decreasing function of the laser energy. Also, it appears that the electron temperature, the plasma density and radius, and the conduction of heat across the plasma boundaries play major roles in the capacity of the laser-created plasma to trigger streamers. The results of the model are compared with the available experimental data.

Energetic protons generated by ultrahigh contrast laser pulses interacting with ultrathin targets

A regime of laser acceleration of protons, which relies on the interaction of ultrahigh contrast laser pulses with ultrathin targets, has been validated using experiments and simulations. Proton beams were accelerated to a maximum energy of ∼7.3MeV from targets as thin as 30nm irradiated at 1018Wcm−2μm2 (1J, 320fs) with an estimated peak laser pulse to pedestal intensity contrast ratio of 1011. This represents nearly a tenfold increase in proton energy compared to the highest energies obtainable using non contrast enhanced pulses and thicker targets (>5μm) at the same intensity. To obtain similar proton energy with thicker targets and the same laser pulse duration, a much higher laser intensity (i.e., above 1019Wcm−2μm2) is required. The simulations are in close agreement with the experimental results, showing efficient electron heating compared to the case of thicker targets. Rapid target expansion, allowing laser absorption in density gradients, is key to enhanced electron heating and ion acceleration i...

Guiding large-scale spark discharges with ultrashort pulse laser filaments

Using the nonlinear propagation properties of ultrashort laser pulses in air, we were able to produce long ionized filaments that served to guide spark discharges. With a laser pulse energy of 20 mJ, one or two ionized filaments were created and could guide streamer discharges over 2 m air gaps, where the electric field was fairly uniform and had an average value of 0.6 MV/m. Such a guiding effect was observed for times of 1–3 μs after the laser pulse created the ionized filaments. Longer delays (10–15 μs) were recorded at higher laser pulse energy, with a larger number of filaments. Images of the early stages of the discharge of a uniform air gap show that the laser-produced ionized filaments do not initiate the discharge process but act rather as preferred channels where the leader growth is accelerated. In the end, these straight conductive channels carry the arc current as the voltage in the gap breaks down.