Complete Characterization of Light Waves using Attosecond Pulses

The most direct way to probe the strength of an electric field, is to measure the force that exerts to a charged particle. For a time varying field, charge placement within an interval substantially shorter than the characteristic period of variation of the field is essential for sampling its temporal evolution. Employing such a scheme to track the field variation of light waves that changes its direction 1015 times per second, charge release shall be confined within a fraction of a femtosecond. In this thesis, the complete characterization of a light pulse is demonstrated experimentally for the first time by probing its field variation using a 250 attosecond electron burst. Such an ultrafast charge probe, can be generated by the impulsive ionization of atoms, using an XUV attosecond pulse precisely synchronized with the light waveform to be characterized. The technique allows access to the instantaneous value of the electric field of IR, visible, or UV light and thereby opens the door for the synthesis of controlled, extremely broadband and arbitrarily shaped light waveforms. The above experiments, are presented along with critical pertinent developments on the generation of few-cycle phase-controlled light waveforms and their subsequent exploitation, for the generation of isolated XUV attosecond pulses. Precisely characterized and controlled light fields and XUV attosecond pulses employed in combination, hold the promise for probe and control of elementary processes evolving on an attosecond time scale

Sub-Cycle Strong-Field Interferometry

A nonlinear interferometry scheme is described theoretically to induce and resolve electron wave- function beating on time scales shorter than the optical cycle of the time-delayed pump and probe pulses. By employing two moderately intense few-cycle laser fields with a stable carrier-envelope phase, a large range of the entire electronic level structure of a quantum system can be retrieved. In contrast to single-photon excitation schemes, the retrieved electronic states include levels that are both dipole- and non-dipole-accessible from the ground electronic state. The results show that strong-field interferometry can reveal both high-resolution and broad-band spectral information at the same time with important consequences for quantum-beat spectroscopy on attosecond or even shorter time scales.Comment: first submitted on April 19, 201

Genetic optimization of attosecond-pulse generation in light-field synthesizers

We demonstrate control over attosecond pulse generation and shaping by numerically optimizing the synthesis of few-cycle to sub-cycle driver waveforms. The optical waveform synthesis takes place in an ultrabroad spectral band covering the ultraviolet-infrared domain. These optimized driver waves are used for ultrashort single and double attosecond pulse production (with tunable separation) revealing the potentials of the light wave synthesizer device demonstrated by Wirth et al. [Science 334, 195 (2011)]. The results are also analyzed with respect to attosecond pulse propagation phenomena

Attosecond control of electrons emitted from a nanoscale metal tip

Attosecond science is based on steering of electrons with the electric field of well-controlled femtosecond laser pulses. It has led to, for example, the generation of XUV light pulses with a duration in the sub-100-attosecond regime, to the measurement of intra-molecular dynamics by diffraction of an electron taken from the molecule under scrutiny, and to novel ultrafast electron holography. All these effects have been observed with atoms or molecules in the gas phase. Although predicted to occur, a strong light-phase sensitivity of electrons liberated by few-cycle laser pulses from solids has hitherto been elusive. Here we show a carrier-envelope (C-E) phase-dependent current modulation of up to 100% recorded in spectra of electrons laser-emitted from a nanometric tungsten tip. Controlled by the C-E phase, electrons originate from either one or two sub-500as long instances within the 6-fs laser pulse, leading to the presence or absence of spectral interference. We also show that coherent elastic re-scattering of liberated electrons takes place at the metal surface. Due to field enhancement at the tip, a simple laser oscillator suffices to reach the required peak electric field strengths, allowing attosecond science experiments to be performed at the 100-Megahertz repetition rate level and rendering complex amplified laser systems dispensable. Practically, this work represents a simple, exquisitely sensitive C-E phase sensor device, which can be shrunk in volume down to ~ 1cm3. The results indicate that the above-mentioned novel attosecond science techniques developed with and for atoms and molecules can also be employed with solids. In particular, we foresee sub-femtosecond (sub-) nanometre probing of (collective) electron dynamics, such as plasmon polaritons, in solid-state systems ranging in size from mesoscopic solids via clusters to single protruding atoms.Comment: Final manuscript version submitted to Natur

Carrier-envelope phase effects on the strong-field photoemission of electrons from metallic nanostructures

Sharp metallic nanotapers irradiated with few-cycle laser pulses are emerging as a source of highly confined coherent electron wavepackets with attosecond duration and strong directivity. The possibility to steer, control or switch such electron wavepackets by light is expected to pave the way towards direct visualization of nanoplasmonic field dynamics and real-time probing of electron motion in solid state nanostructures. Such pulses can be generated by strong-field induced tunneling and acceleration of electrons in the near-field of sharp gold tapers within one half-cycle of the driving laser field. Here, we show the effect of the carrier-envelope phase of the laser field on the generation and motion of strong-field emitted electrons from such tips. This is a step forward towards controlling the coherent electron motion in and around metallic nanostructures on ultrashort length and time scales

The direct evaluation of attosecond chirp from a streaking measurement

We derive an analytical expression, from classical electron trajectories in a laser field, that relates the breadth of a streaked photoelectron spectrum to the group-delay dispersion of an isolated attosecond pulse. Based on this analytical expression, we introduce a simple, efficient and robust procedure to instantly extract the attosecond pulse's chirp from the streaking measurement.Comment: 4 figure

Attosecond double-slit experiment

A new scheme for a double-slit experiment in the time domain is presented. Phase-stabilized few-cycle laser pulses open one to two windows (``slits'') of attosecond duration for photoionization. Fringes in the angle-resolved energy spectrum of varying visibility depending on the degree of which-way information are observed. A situation in which one and the same electron encounters a single and a double slit at the same time is discussed. The investigation of the fringes makes possible interferometry on the attosecond time scale. The number of visible fringes, for example, indicates that the slits are extended over about 500as.Comment: 4 figure