Éric Bisson

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.

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.

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+.

Isotope Effect in the three Break-up Channels of the Acetylene Cation

The dynamics and the isotope effect on the symmetric (CH++CH+), the deprotonation (C2H++H+), and the isomerization channel (CH2 ++C+) is studied systematically by pump (four 266 nm photons) probe (800nm) excitation.

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.

Sub two-cycle pulse compression at 1.8 µm with bulk material

A simple scheme for generating 0.4 mJ 11.5 fs pulses at 1.8 µm is presented. Optical parametric amplified pulses were spectrally broadened in a hollow-core fiber and subsequently compressed by utilizing linear propagation through bulk material.