Stefan Roither

Attosecond-recollision-controlled selective fragmentation of polyatomic molecules.

Control over various fragmentation reactions of a series of polyatomic molecules (acetylene, ethylene, 1,3-butadiene) by the optical waveform of intense few-cycle laser pulses is demonstrated experimentally. We show both experimentally and theoretically that the responsible mechanism is inelastic ionization from inner-valence molecular orbitals by recolliding electron wave packets, whose recollision energy in few-cycle ionizing laser pulses strongly depends on the optical waveform. Our work demonstrates an efficient and selective way of predetermining fragmentation and isomerization reactions in polyatomic molecules on subfemtosecond time scales.

Effect of laser parameters on ultrafast hydrogen migration in methanol studied by coincidence momentum imaging.

The effect of intensity, duration, and polarization of ultrashort laser pulses (795 nm, 40-100 fs, and 0.15-1.5 × 10(15) W/cm(2)) on the hydrogen migration in methanol is systematically investigated using Coulomb explosion coincidence momentum imaging. The ratio of the ion yield obtained for the migration pathway CH(3)OH(2+) → CH(2)(+) + OH(2)(+) with respect to the sum of the yields obtained for the migration pathway and for the nonmigration pathway CH(3)OH(2+) → CH(3)(+) + OH(+) exhibits a small (10-20%) but clear dependence on laser pulse properties, that is, the ratio decreases as the laser peak intensity increases but increases when the pulse duration increases as well as when the laser polarization is changed from linear to circular.

Two-proton migration in 1,3-butadiene in intense laser fields

Ultrafast proton migration in 1,3-butadiene in an intense laser field (40 fs, 4.5 × 10(14) W cm(-2)) is investigated by using Coulomb explosion coincidence momentum imaging. The spatial distribution maps of a migrating proton reconstructed for the two three-body Coulomb explosion pathways, C(4)H(6)(3+)→ H(+) + CH(3)(+) + C(3)H(2)(+) and C(4)H(6)(3+)→ H(+) + C(2)H(+) + C(2)H(4)(+), reveal that two protons migrate within a 1,3-butadiene molecule, prior to the three body decomposition.

Polarization of terahertz radiation from laser generated plasma filaments

An analysis of the polarization of terahertz (THz) radiation from a laser-induced plasma source is presented. THz emission is achieved by mixing a laser pulse with its second harmonic after focusing through a β-BaB2O4 (β-BBO) crystal. Numerical calculations, based on the nonlinear four-wave mixing model and the microscopic polarization model, are compared with experimental results. The main focus lies on the study of the dependence of THz polarization on the polarization and relative phase of the incident fundamental and second-harmonic pulses. We show that the modulation of the fundamental pulse by the BBO crystal has to be taken into account in order to describe experimental observations. By including the finite extension of the plasma and considering cross- and self-phase modulation of the two-color pump pulse, we are able to explain the observed ellipticity of the THz pulse as well as the orientation of the polarization axis.

Sagnac interferometric multipass loop amplifier

We propose and investigate experimentally an interferometrically stable, polarization-selective pulse multiplexing scheme for direct laser amplification of picosecond pulses. The basic building block of this scheme is a Sagnac loop which allows for a straightforward scaling of the pulse-multiplexing scheme. Switching the amplifier from single-pulse amplification to burst mode increases extraction efficiency, reduces parasitic non-linearities in the gain medium and allows for higher output energies. Time-frequency analysis of the amplified output pulses demonstrates the viability of this approach.

Path-selective investigation of intense laser-pulse-induced fragmentation dynamics in triply charged 1,3-butadiene

We experimentally studied proton ejection in the three-body fragmentation of triply charged 1,3-butadiene molecules prepared by intense ultrashort laser pulses using coincidence momentum imaging. The break-up dynamics along the four possible paths that a final set of three fragments can be reached is investigated for the three different fragmentation channels that are analysed. It is found that for each channel the two dominant paths are (i) proton ejection from the triply charged ion and (ii) a sequential path, where the proton is ejected from the doubly charged ion during the second fragmentation step. Based on the measured three-body momentum correlations and accompanying numerical simulations, we discuss whether the fragmentation dynamics, where the proton is ejected from the triply charged ion, proceeds concertedly or sequentially. We also investigate the dependence of the fragmentation dynamics on the intensity and polarization state of the laser pulse.

Angular encoding in attosecond recollision

We describe a general concept of using the spatial information encoded in the time-dependent polarization of high harmonic radiation generated by orthogonally polarized two-color laser fields. The main properties of recolliding electron wave packets driven by such fields are reviewed. It is shown that in addition to the recollision energy the angle of recollision of such wave packets, which is directly mapped onto the polarization direction of the emitted high harmonic radiation, varies on a sub-laser-cycle time-scale. Thus, a mapping between the polarization angle and the frequency of the emitted radiation is established on an attosecond time scale. While the polarization angle encodes the spatial properties of the recollision process, the frequency is linked to time via the well-known dispersion relations of high harmonic generation. Based on these principles, we show that in combination with polarization selective detection the use of orthogonally polarized drive pulses for high harmonic generation permit one to construct spatially resolved attosecond measurements. Here, we present two examples of possible applications: (i) a method for isolating a single attosecond pulse from an attosecond pulse train which is more efficient than the cut-off selection method, and (ii) a technique for orbital tomography of molecules with attosecond resolution.

Laser-sub-cycle two-dimensional electron-momentum mapping using orthogonal two-color fields

We study laser-sub-cycle control over electron trajectories concomitantly in space and time using orthogonally polarized two-color laser fields. We compare experimental photoelectron spectra of neon recorded by coincidence momentum imaging with photoelectron spectra obtained by semiclassical and numerical solutions of the time-dependent Schrodinger equation. We find that a resolution of a quarter optical cycle in the photoelectron trajectories can be achieved. It is shown that depending on their sub-cycle birth time the trajectories of photoelectrons are affected differently by the ions Coulomb field.

Probing the influence of the Coulomb field on atomic ionization by sculpted two-color laser fields

Interpretation of electron or photon spectra obtained with strong laser pulses that may carry attosecond dynamical and Angstrom structural information about atoms or molecules usually relies on variants of the strong-field approximation (SFA) within which the influence of the Coulomb potential on the electron trajectory is neglected. We employ two-color sculpted laser fields to experimentally tune and probe the influence of the Coulomb field on the strong-field-driven wavepacket as observed by two-dimensional electron and ion momentum spectra. By comparison of measured spectra with predictions of the three-dimensional time-dependent Schrodinger equation as well as the quasi-classical limit of the SFA, the strong-field classical trajectory model, we are able to trace back the influence of the Coulomb field to the timing of the wavepacket release with sub-cycle precision.

Duration of an intense laser pulse can determine the breakage of multiple chemical bonds.

Control over the breakage of a certain chemical bond in a molecule by an ultrashort laser pulse has been considered for decades. With the availability of intense non-resonant laser fields it became possible to pre-determine femtosecond to picosecond molecular bond breakage dynamics by controlled distortions of the electronic molecular system on sub-femtosecond time scales using field-sensitive processes such as strong-field ionization or excitation. So far, all successful demonstrations in this area considered only fragmentation reactions, where only one bond is broken and the molecule is split into merely two moieties. Here, using ethylene (C2H4) as an example, we experimentally investigate whether complex fragmentation reactions that involve the breakage of more than one chemical bond can be influenced by parameters of an ultrashort intense laser pulse. We show that the dynamics of removing three electrons by strong-field ionization determines the ratio of fragmentation of the molecular trication into two respectively three moieties. We observe a relative increase of two-body fragmentations with the laser pulse duration by almost an order of magnitude. Supported by quantum chemical simulations we explain our experimental results by the interplay between the dynamics of electron removal and nuclear motion.