Mathieu Giguère

Compression of 1.8 μm laser pulses to sub two optical cycles with bulk material

We demonstrate a simple scheme to generate 0.4 mJ 11.5 fs laser pulses at 1.8 μm. Optical parametrically amplified pulses are spectrally broadened by nonlinear propagation in an argon-filled hollow-core fiber and subsequently compressed to 1.9 optical cycles by linear propagation through bulk material in the anomalous dispersion regime. This pulse compression scheme is confirmed through numerical simulations.

High harmonic generation with long-wavelength few-cycle laser pulses

We report the extension of hollow-core fibre pulse compression to longer wavelengths. High-energy multi-cycle infrared pulses are generated via optical parametric amplification and subsequently broadened in the fibre. 2.5-cycle pulses at the Signal wavelength (1.4 ?m) and 1.6-cycle pulses at the Idler wavelength (1.8 ?m) in the sub-millijoule regime have been generated. New compression schemes can be applied at 1.8 ?m and beyond. In this manner, 1.6-cycle carrier envelope phase stable pulses were generated by linear propagation in the anomalous dispersion regime of bulk glass which surprisingly enables compression below its third-order dispersion limit. Furthermore, a dispersion-free way of controlling the carrier envelope phase is demonstrated. Moreover, we experimentally confirm the increase in high-harmonic cut-off energy with driving laser wavelength and demonstrate the beneficial effect of few-cycle pulses which enable higher saturation intensities on target compared to multi-cycle pulses. It will be an ideal tool for future synthesis of isolated attosecond pulses in the sub-keV regime. With this laser source, we revealed for the first time multi-electron effects in high harmonic generation in xenon.

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.

Pulse compression of submillijoule few-optical-cycle infrared laser pulses using chirped mirrors

We report generation of 400 microJ, 13.1 fs, 1425 nm optical parametric amplifier laser pulses. Spectral broadening of a 100 Hz optical parametric amplifier laser source is achieved by self-phase modulation in an argon-filled hollow-core fiber, and dispersion compensation is performed using chirped mirrors. This laser source will be useful for ultrafast time-resolved molecular orbital tomography.

Widely tunable mid-infrared generation via frequency conversion in semiconductor waveguides

Phase matching in a multilayer AlGaAs waveguide is used to generate mid-IR (7.5-8.5 μm) light through difference frequency generation (DFG) between a 1550 nm pump and 1950 nm signal. This represents the longest wavelength generated through DFG in a 2D waveguide mode in a semiconductor waveguide. It was produced with an efficiency of 1.2×10(-4) %/W in a 1 mm long sample. The process is shown to be tunable across >2 μm through appropriate tuning of the input pump and signal wavelengths and/or waveguide geometry, and is therefore a viable platform for monolithic, tunable, mid-IR sources.

N2O ionization and dissociation dynamics in intense femtosecond laser radiation, probed by systematic pulse length variation from 7 to 500 fs

We have made a series of measurements, as a function of pulse duration, of ionization and fragmentation of the asymmetric molecule N2O in intense femtosecond laser radiation. The pulse length was varied from 7 fs to 500 fs with intensity ranging from 4 × 10(15) to 2.5 × 10(14) W∕cm(2). Time and position sensitive detection allows us to observe all fragments in coincidence. By representing the final dissociation geometry with Dalitz plots, we can identify the underlying breakup dynamics. We observe for the first time that there are two stepwise dissociation pathways for N2O(3+): (1) N2O(3+) → N(+) + NO(2+) → N(+) + N(+) + O(+) and (2) N2O(3+) → N2 (2+) + O(+) → N(+) + N(+) + O(+) as well as one for N2O(4+) → N(2+) + NO(2+) → N(2+) + N(+) + O(+). The N2 (2+) stepwise channel is suppressed for longer pulse length, a phenomenon which we attribute to the influence which the structure of the 3+ potential has on the dissociating wave packet propagation. Finally, by observing the total kinetic energy released for each channel as a function of pulse duration, we show the increasing importance of charge resonance enhanced ionization for channels higher than 3+.

Comparing Coulomb explosion dynamics of multiply charged triatomic molecules after ionization by highly charged ion impact and few cycle femtosecond laser pulses

Recent experiments using highly charged ions (HCI) at Tokyo Metropolitan University and few cycle laser pulses at the advanced laser light source have centered on multiply ionizing carbonyl sulfide to form charge states from 3 + to 7 + . By measuring the kinetic energy release during subsequent break up and comparing with previous results from HCI impact on CO2 we can see a pattern emerging which implies that shorter laser pulses than the current sub 7 fs standard could lead to higher kinetic energy release than expected from Coulomb explosion.

Tabletop imaging using 266nm femtosecond laser pulses, for characterization of structural evolution in, single molecule, chemical reactions

We have demonstrated a generally applicable tabletop approach utilizing a 266nm femtosecond laser pulse pump, 800nm pulse probe, coupled with Coulomb explosion imaging (CEI). We have investigated two simple chemical reactions in C2H2+ simultaneously: proton transfer and C=C bond-breaking, triggered by multiphoton ionization to excited states. Too and fro proton migration results are in excellent agreement with new ab initio trajectory simulations which predict isomerization timescales and pathways.

N2O ionization and dissociation dynamics in intense few cycle femtosecond laser radiation

Using few cycle pulses, uniform-electric-field-ion imaging spectrometer and Dalitz plotting, we can identify two new stepwise processes, in the dissociation of the 3+ and 4+ states of N2O in intense few cycle pulses at 4 × 1015 Wcm−2. We observe suppression of selective channels at longer pulse length, which we attribute to molecular dynamics on the 2+ state and the shape of the 3+ potential, which influences propagation of the dissociating wave packet.

A scaling mechanism for increasing the terahertz emission from ionization of air

A significant enhancement of the terahertz generation efficiency via two-color laser-induced air ionization, up to 10-3, is observed with increasing pump wavelength. Terahertz peak fields up to 4.4 MV/cm were obtained using 400 μJ pulse energy.