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Ultrashort electron pulses are crucial for time-resolved electron diffraction and microscopy of fundamental light-matter interaction. In this work, we study experimentally and theoretically the generation and characterization of attosecond electron pulses by optical-field-driven compression and streaking at dielectric or absorbing interaction elements. The achievable acceleration and deflection gradient depends on the laser-electron angle, the lasers electric and magnetic field directions and the foil orientation. Electric and magnetic fields have similar contributions to the final effect and both need to be considered. Experiments and theory agree well and reveal the optimum conditions for highly efficient, velocity-matched electron-field interactions in longitudinal or transverse direction. We find that metallic membranes are optimum for light-electron control at mid-infrared or terahertz wavelengths, but dielectric membranes are excel in the visible/near-infrared regimes and are therefore ideal for the formation of attosecond electron pulses.
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Attosecond pulses are fundamental for the investigation of valence and core-electron dynamics on their natural timescale. At present the reproducible generation and characterisation of attosecond waveforms has been demonstrated only through the process of high-order harmonic generation. Several methods for the shaping of attosecond waveforms have been proposed, including metallic filters, multilayer mirrors and manipulation of the driving field. However, none of these approaches allow for the flexible manipulation of the temporal characteristics of the attosecond waveforms, and they suffer from the low conversion efficiency of the high-order harmonic generation process. Free Electron Lasers, on the contrary, deliver femtosecond, extreme ultraviolet and X-ray pulses with energies ranging from tens of $mathrm{mu}$J to a few mJ. Recent experiments have shown that they can generate sub-fs spikes, but with temporal characteristics that change shot-to-shot. Here we show the first demonstration of reproducible generation of high energy ($mathrm{mu}$J level) attosecond waveforms using a seeded Free Electron Laser. We demonstrate amplitude and phase manipulation of the harmonic components of an attosecond pulse train in combination with a novel approach for its temporal reconstruction. The results presented here open the way to perform attosecond time-resolved experiments with Free Electron Lasers.
The generation of coherent light pulses in the extreme ultraviolet (XUV) spectral region with attosecond pulse durations constitutes the foundation of the field of attosecond science. Twenty years after the first demonstration of isolated attosecond pulses, they continue to be a unique tool enabling the observation and control of electron dynamics in atoms, molecules and solids. It has long been identified that an increase in the repetition rate of attosecond light sources is necessary for many applications in atomic and molecular physics, surface science, and imaging. Although high harmonic generation (HHG) at repetition rates exceeding 100 kHz, showing a continuum in the cut-off region of the XUV spectrum was already demonstrated in 2013, the number of photons per pulse was insufficient to perform pulse characterisation via attosecond streaking, let alone to perform a pump-probe experiment. Here we report on the generation and full characterisation of XUV attosecond pulses via HHG driven by near-single-cycle pulses at a repetition rate of 100 kHz. The high number of 10^6 XUV photons per pulse on target enables attosecond electron streaking experiments through which the XUV pulses are determined to consist of a dominant single attosecond pulse. These results open the door for attosecond pump-probe spectroscopy studies at a repetition rate one or two orders of magnitude above current implementations.
We present a method to control photodissociation by manipulating the bond softening mechanism occurring in strong shaped laser fields, by varying the chirp sign and magnitude of an ultra-short laser pulse. Manipulation of bond-softening is experimentally demonstrated for strong field (795 nm, 10^12 - 10^13 W/cm^2) photodissociation of H2+, exhibiting substantial increase of dissociation by positively chirped pulses with respect to both negatively chirped and transform limited pulses. The measured kinetic energy release and angular distributions are used to quantify the degree of control of dissociation. The control mechanism is attributed to the interplay of dynamic alignment and chirped light induced potential curves.
Interference between multiple distinct paths is a defining property of quantum physics, where paths may involve actual physical trajectories, as in interferometry, or transitions between different internal (e.g. spin) states, or both. A hallmark of quantum coherent evolution is the possibility to interact with a system multiple times in a phase-preserving manner. This principle underpins powerful multi-dimensional optical and nuclear magnetic resonance spectroscopies and related techniques, including Ramseys method of separated oscillatory fields used in atomic clocks. Previously established for atomic, molecular and quantum dot systems, recent developments in the optical quantum state preparation of free electron beams suggest a transfer of such concepts to the realm of ultrafast electron imaging and spectroscopy. Here, we demonstrate the sequential coherent interaction of free electron states with two spatially separated, phase-controlled optical near-fields. Ultrashort electron pulses are acted upon in a tailored nanostructure featuring two near-field regions with anisotropic polarization response. The amplitude and relative phase of these two near-fields are independently controlled by the incident polarization state, allowing for constructive and destructive quantum interference of the subsequent interactions. Future implementations of such electron-light interferometers may yield unprecedented access to optically phase-resolved electronic dynamics and dephasing mechanisms with attosecond precision.
High-harmonic generation in two-colour ($omega-2omega$) counter-rotating circularly polarised laser fields opens the path to generate isolated attosecond pulses and attosecond pulse trains with controlled ellipticity. The generated harmonics have alternating helicity, and the ellipticity of the generated attosecond pulse depends sensitively on the relative intensities of two adjacent, counter-rotating harmonic lines. For the $s$-type ground state, such as in Helium, the successive harmonics have nearly equal amplitude, yielding isolated attosecond pulses and attosecond pulse trains with linear polarisation, rotated by 120$^{{circ}}$ from pulse to pulse. In this work, we suggest a solution to overcome the limitation associated with the $s$-type ground state. It is based on modifying the three propensity rules associated with the three steps of the harmonic generation process: ionisation, propagation, and recombination. We control the first step by seeding high harmonic generation with XUV light tuned well below the ionisation threshold, which generates virtual excitations with the angular momentum co-rotating with the $omega$-field. We control the propagation step by increasing the intensity of the $omega$-field relative to the $2omega$-field, further enhancing the chance of the $omega$-field being absorbed versus the $2omega$-field, thus favouring the emission co-rotating with the seed and the $omega-$field. We demonstrate our proposed control scheme using Helium atom as a target and solving time-dependent Schr{o}dinger equation in two and three-dimensions.
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