Nicolas Thiré

Linking high harmonics from gases and solids

When intense light interacts with an atomic gas, recollision between an ionizing electron and its parent ion creates high-order harmonics of the fundamental laser frequency. This sub-cycle effect generates coherent soft X-rays and attosecond pulses, and provides a means to image molecular orbitals. Recently, high harmonics have been generated from bulk crystals, but what mechanism dominates the emission remains uncertain. To resolve this issue, we adapt measurement methods from gas-phase research to solid zinc oxide driven by mid-infrared laser fields of 0.25 volts per ångström. We find that when we alter the generation process with a second-harmonic beam, the modified harmonic spectrum bears the signature of a generalized recollision between an electron and its associated hole. In addition, we find that solid-state high harmonics are perturbed by fields so weak that they are present in conventional electronic circuits, thus opening a route to integrate electronics with attosecond and high-harmonic technology. Future experiments will permit the band structure of a solid to be tomographically reconstructed.

All-Optical Reconstruction of Crystal Band Structure

The band structure of matter determines its properties. In solids, it is typically mapped with angle-resolved photoemission spectroscopy, in which the momentum and the energy of incoherent electrons are independently measured. Sometimes, however, photoelectrons are difficult or impossible to detect. Here we demonstrate an all-optical technique to reconstruct momentum-dependent band gaps by exploiting the coherent motion of electron-hole pairs driven by intense midinfrared femtosecond laser pulses. Applying the method to experimental data for a semiconductor ZnO crystal, we identify the split-off valence band as making the greatest contribution to tunneling to the conduction band. Our new band structure measurement technique is intrinsically bulk sensitive, does not require a vacuum, and has high temporal resolution, making it suitable to study reactions at ambient conditions, matter under extreme pressures, and ultrafast transient modifications to band structures.

Tabletop imaging of structural evolutions in chemical reactions demonstrated for the acetylene cation

The introduction of femto-chemistry has made it a primary goal to follow the nuclear and electronic evolution of a molecule in time and space as it undergoes a chemical reaction. Using Coulomb Explosion Imaging, we have shot the first high-resolution molecular movie of a to and fro isomerization process in the acetylene cation. So far, this kind of phenomenon could only be observed using vacuum ultraviolet light from a free-electron laser. Here we show that 266 nm ultrashort laser pulses are capable of initiating rich dynamics through multiphoton ionization. With our generally applicable tabletop approach that can be used for other small organic molecules, we have investigated two basic chemical reactions simultaneously: proton migration and C=C bond breaking, triggered by multiphoton ionization. The experimental results are in excellent agreement with the timescales and relaxation pathways predicted by new and quantitative ab initio trajectory simulations.

Multioctave infrared supercontinuum generation in large-core As2S3 fibers

We report on infrared supercontinuum (SC) generation through laser filamentation and subsequent nonlinear propagation in a step-index As2S3 fiber. The 100 μm core and high-purity As2S3 fiber used exhibit zero-dispersion wavelength around 4.5 μm, a mid-infrared background loss of 0.2  dB/m, and a maximum loss of only 0.55  dB/m at the S-H absorption peak around 4.05 μm. When pumping with ultrashort laser pulses slightly above the S-H absorption band, broadband infrared supercontinua were generated with a 20 dB spectral flatness spanning from 1.5 up to 7 μm. The efficiency and spectral shape of the SC produced by ultrashort pulses in large-core As2S3 fiber are mainly determined by its dispersion, the S-H contaminant absorption, and the mid-infrared nonlinear absorption.

High-order harmonic spectroscopy of the Cooper minimum in argon: Experimental and theoretical study

We study the Cooper minimum in high-order-harmonic generation from argon atoms by using long wavelength laser pulses. We find that the minimum in high-order-harmonic spectra is systematically shifted with respect to total photoionization cross section measurements. We use a semiclassical theoretical approach based on classical trajectory Monte Carlo and quantum electron scattering methods to model the experiment. Our study reveals that the shift between photoionization and high-order-harmonic emission is due to several effects: the directivity of the recombining electrons and emitted polarization, and the shape of the recolliding electron wave packet.

Mid-infrared supercontinuum generation in fluoroindate fiber

We report the generation of mid-infrared supercontinua in a step-index fluoroindate-based fiber. The large core of the fluoroindate fiber allows the guiding of multiwatt laser power over a broad spectral range. These fibers exhibit zero dispersion at 1.83 μm, minimal loss of 0.1 dB/m at 3.2 μm up to only 0.8 dB/m at 5 μm. These specifications enable mid-infrared supercontinuum generation and propagation with low loss. By using mid-infrared ultrashort laser pulses from an optical parametric amplifier, we demonstrate generation of a 20 dB spectral flatness supercontinua from 2.7 to 4.7 μm in the fluoroindate fiber, which is twice the spectral broadening compared to a ZBLAN fiber under similar conditions.

Inhomogeneous high harmonic generation in krypton clusters.

High order harmonic generation from clusters is a controversial topic: conflicting theories exist, with different explanations for similar experimental observations. From an experimental point of view, separating the contributions from monomers and clusters is challenging. By performing a spectrally and spatially resolved study in a controlled mixture of clusters and monomers, we are able to isolate a region of the spectrum where the emission purely originates from clusters. Surprisingly, the emission from clusters is depolarized, which is the signature of statistical inhomogeneous emission from a low-density source. The harmonic response to laser ellipticity shows that this generation is produced by a new recollisional mechanism, which opens the way to future theoretical studies.

10 mJ 5-cycle pulses at 1.8 μm through optical parametric amplification

We report the generation of 10 mJ, 5-cycle pulses at 1.8 μm (30 fs) at 100 Hz repetition rate using an optical parametric amplifier pumped by a high energy Titanium-Sapphire laser system (total energy of 23 mJ for Signal and Idler). This is the highest reported peak power (0.33 TW) in the infrared spectral range. This high-energy long wavelength laser source is well suited for driving various nonlinear optical phenomena such as high harmonic generation for high flux ultrafast soft X-ray pulses.

0.42 TW 2-cycle pulses at 1.8 μm via hollow-core fiber compression

By employing pulse compression with a stretched hollow-core fiber, we generated 2-cycle pulses at 1.8 μm (12 fs) carrying 5 mJ of pulse energy at 100 Hz repetition rate. This energy scaling in the mid-infrared spectral range was achieved by lowering the intensity in a loose focusing condition, thus suppressing the ionization induced losses. The correspondingly large focus was coupled into a hollow-core fiber of 1 mm inner diameter, operated with a pressure gradient to further reduce detrimental nonlinear effects. The required amount of self-phase modulation for spectral broadening was obtained over 3 m of propagation distance.

Coherent control of D2/H2 dissociative ionization by a mid-infrared two-color laser field

Steering the electrons during an ultrafast photo-induced process in a molecule influences the chemical behavior of the system, opening the door to the control of photochemical reactions and photobiological processes. Electrons can be efficiently localized using a strong laser field with a well-designed temporal shape of the electric component. Consequently, many experiments have been performed with laser sources in the near-infrared region (800 nm) in the interest of studying and enhancing the electron localization. However, due to its limited accessibility, the mid-infrared (MIR) range has barely been investigated, although it allows to efficiently control small molecules and even more complex systems. To push further the manipulation of basic chemical mechanisms, we used a MIR two-color (1800 and 900 nm) laser field to ionize H2 and D2 molecules and to steer the remaining electron during the photo-induced dissociation. The study of this prototype reaction led to the simultaneous control of four fragmentation channels. The results are well reproduced by a theoretical model solving the time-dependent Schrodinger equation for the molecular ion, identifying the involved dissociation mechanisms. By varying the relative phase between the two colors, asymmetries (i.e., electron localization selectivity) of up to 65% were obtained, corresponding to enhanced or equivalent levels of control compared to previous experiments. Experimentally easier to implement, the use of a two-color laser field leads to a better electron localization than carrier-envelope phase stabilized pulses and applying the technique in the MIR range reveals more dissociation channels than at 800 nm.