No Arabic abstract
The use of strong-field (i.e. intensities in excess of 10^13 Wcm-2) few-cycle ultrafast (durations of 10 femtoseconds or less) laser pulses to create, manipulate and image vibrational wavepackets is investigated. Quasi-classical modelling of the initial superposition through tunnel ionization, wavepacket modification by nonadiabatically altering the nuclear environment via the transition dipole and the Stark effect, and measuring the control outcome by fragmenting the molecule is detailed. The influence of the laser intensity on strong-field ultrafast wavepacket control is discussed in detail: by modifying the distribution of laser intensities imaged, we show that focal conditions can be created that give preference to this three-pulse technique above processes induced by the pulses alone. An experimental demonstration is presented, and the nuclear dynamics inferred by the quasi-classical model discussed. Finally, we present the results of a systematic investigation of a dual-control pulse scheme, indicating that single vibrational states should be observable with high fidelity, and the populated state defined by varying the arrival time of the two control pulses. The relevance of such strong-field coherent control methods to the manipulation of electron localization and attosecond science is discussed.
We analyze the role of the difference between the central frequencies of the spectral distributions of the vector potential and the electric field of a short laser pulse. The frequency shift arises when the electric field is determined as the derivative of the vector potential to ensure that both quantities vanish at the beginning and end of the pulse. We derive an analytical estimate of the frequency shift and show how it affects various light induced processes, such as excitation, ionization and high harmonic generation. Since observables depend on the frequency spectrum of the electric field, the shift should be taken into account when setting the central frequency of the vector potential to avoid potential misinterpretation of numerical results for processes induced by few-cycle pulses.
The laser-induced fragmentation dynamics of this most fundamental polar molecule HeH$^+$ are measured using an ion beam of helium hydride and an isotopologue at various wavelengths and intensities. In contrast to the prevailing interpretation of strong-field fragmentation, in which stretching of the molecule results primarily from laser-induced electronic excitation, experiment and theory for nonionizing dissociation, single ionization and double ionization both show that the direct vibrational excitation plays the decisive role here. We are able to reconstruct fragmentation pathways and determine the times at which each ionization step occurs as well as the bond length evolution before the electron removal. The dynamics of this extremely asymmetric molecule contrast the well-known symmetric systems leading to a more general picture of strong-field molecular dynamics and facilitating interpolation to systems between the two extreme cases.
Isolated attosecond pulses (IAPs) produced through laser-driven high-harmonic generation (HHG) hold promise for unprecedented insight into biological processes via attosecond x-ray diffraction with tabletop sources. However, efficient scaling of HHG towards x-ray energies has been hampered by ionization-induced plasma generation impeding the coherent buildup of high-harmonic radiation. Recently, it has been shown that these limitations can be overcome in the so-called overdriven regime where ionization loss and plasma dispersion strongly modify the driving laser pulse over small distances, albeit without demonstrating IAPs. Here, we report on experiments comparing the generation of IAPs in argon and neon at 80 eV via attosecond streaking measurements. Contrasting our experimental results with numerical simulations, we conclude that IAPs in argon are generated through ionization-induced transient phase-matching gating effective over distances on the order of 100 $mu$m. We show that the decay of the intensity and blue-shift due to plasma defocussing are crucial for allowing phase-matching close to the XUV cutoff at high plasma densities. We perform simulations for different gases and wavelengths and show that the mechanism is important for the phase-matching of long-wavelength, tightly-focused laser beams in high-pressure gas targets, which are currently being employed for scaling isolated attosecond pulse generation to x-ray photon energies.
This work describes the first observations of the ionisation of neon in a metastable atomic state utilising a strong-field, few-cycle light pulse. We compare the observations to theoretical predictions based on the Ammosov-Delone-Krainov (ADK) theory and a solution to the time-dependent Schrodinger equation (TDSE). The TDSE provides better agreement with the experimental data than the ADK theory. We optically pump the target atomic species and demonstrate that the ionisation rate depends on the spin state of the target atoms and provide physically transparent interpretation of such a spin dependence in the frameworks of the spin-polarised Hartree-Fock and random-phase approximations.
We report on the unambiguous observation of the sub-cycle ionization bursts in sequential strong-field double ionization of H$_2$ and their disentanglement in molecular frame photoelectron angular distributions. This observation was made possible by the use of few-cycle laser pulses with a known carrier-envelope phase in combination with multi-particle coincidence momentum imaging. The approach demonstrated here will allow sampling of the intramolecular electron dynamics and the investigation of charge-state specific Coulomb-distortions on emitted electrons in polyatomic molecules.