The SwissFEL soft X-ray free-electron laser beamline: Athos.

The SwissFEL soft X-ray free-electron laser (FEL) beamline Athos will be ready for user operation in 2021. Its design includes a novel layout of alternating magnetic chicanes and short undulator segments. Together with the APPLE X architecture of undulators, the Athos branch can be operated in different modes producing FEL beams with unique characteristics ranging from attosecond pulse length to high-power modes.

Time resolved 3D momentum imaging of ultrafast dynamics by coherent VUV-XUV radiation.

We present a new experimental setup for measuring ultrafast nuclear and electron dynamics of molecules after photo-excitation and ionization. We combine a high flux femtosecond vacuum ultraviolet (VUV) and extreme ultraviolet (XUV) source with an internally cold molecular beam and a 3D momentum imaging particle spectrometer to measure electrons and ions in coincidence. We describe a variety of tools developed to perform pump-probe studies in the VUV-XUV spectrum and to modify and characterize the photon beam.

Attosecond Coherent Control of Single and Double Photoionization in Argon.

Ultrafast high harmonic beams provide new opportunities for coherently controlling excitation and ionization processes in atoms, molecules, and materials on attosecond time scales by employing multiphoton two-pathway electron-wave-packet quantum interferences. Here we use spectrally tailored and frequency tuned vacuum and extreme ultraviolet harmonic combs, together with two phase-locked infrared laser fields, to show how the total single and double photoionization yields of argon can be coherently modulated by controlling the relative phases of both optical and electronic-wave-packet quantum interferences. This Letter is the first to apply quantum control techniques to double photoionization, which is a fundamental process where a single, high-energy photon ionizes two electrons simultaneously from an atom.

Bright high-repetition-rate source of narrowband extreme-ultraviolet harmonics beyond 22 eV.

Novel table-top sources of extreme-ultraviolet light based on high-harmonic generation yield unique insight into the fundamental properties of molecules, nanomaterials or correlated solids, and enable advanced applications in imaging or metrology. Extending high-harmonic generation to high repetition rates portends great experimental benefits, yet efficient extreme-ultraviolet conversion of correspondingly weak driving pulses is challenging. Here, we demonstrate a highly-efficient source of femtosecond extreme-ultraviolet pulses at 50-kHz repetition rate, utilizing the ultraviolet second-harmonic focused tightly into Kr gas.

Attosecond vacuum UV coherent control of molecular dynamics.

High harmonic light sources make it possible to access attosecond timescales, thus opening up the prospect of manipulating electronic wave packets for steering molecular dynamics. However, two decades after the birth of attosecond physics, the concept of attosecond chemistry has not yet been realized; this is because excitation and manipulation of molecular orbitals requires precisely controlled attosecond waveforms in the deep UV, which have not yet been synthesized. Here, we present a unique approach using attosecond vacuum UV pulse-trains to coherently excite and control the outcome of a simple chemical reaction in a deuterium molecule in a non-Born-Oppenheimer regime.

Direct visualization of laser-driven electron multiple scattering and tunneling distance in strong-field ionization.

Using a simple model of strong-field ionization of atoms that generalizes the well-known 3-step model from 1D to 3D, we show that the experimental photoelectron angular distributions resulting from laser ionization of xenon and argon display prominent structures that correspond to electrons that pass by their parent ion more than once before strongly scattering. The shape of these structures can be associated with the specific number of times the electron is driven past its parent ion in the laser field before scattering. Furthermore, a careful analysis of the cutoff energy of the structures allows us to experimentally measure the distance between the electron and ion at the moment of tunnel ionization.

Controlling the XUV transparency of helium using two-pathway quantum interference.

Atoms irradiated with combined femtosecond laser and extreme ultraviolet (XUV) fields ionize through multiphoton processes, even when the energy of the XUV photon is below the ionization potential. However, in the presence of two different XUV photons and an intense laser field, it is possible to induce full electromagnetic transparency. Taking helium as an example, the laser field modifies its electronic structure, while the presence of two different XUV photons and the laser field leads to two distinct ionization pathways that can interfere destructively.

Laser-enabled Auger decay in rare-gas atoms.

In rare-gas atoms, Auger decay in which an inner-valence shell ns hole is filled is not energetically allowed. However, in the presence of a strong laser field, a new laser-enabled Auger decay channel can open up to increase the double-ionization yield. This process is efficient at high laser intensities, where an ns hole can be filled within a few femtoseconds of its creation.

Control of electron localization in deuterium molecular ions using an attosecond pulse train and a many-cycle infrared pulse.

We demonstrate an experimental control of electron localization in deuterium molecular ions created and dissociated by the combined action of an attosecond pulse train and a many-cycle infrared (IR) pulse. The attosecond pulse train is synthesized using both even and odd high order harmonics of the driving IR frequency so that it can strobe the IR field once per IR cycle. An asymmetric ejection of the deuterium ions oscillates with the full IR period when the APT-IR time-delay is scanned.

Ion-energy dependence of asymmetric dissociation of D2 by a two-color laser field.

Two-color (800 and 400 nm) short (45 fs) linearly polarized pulses are used to ionize and dissociate D2 into a neutral deuterium atom and a deuteron. The yields and energies of the ions are measured left and right along the polarization vector. As the relative phase of the two colors is varied, strong yield asymmetries are found in the ion-energy regions traditionally identified as bond softening, above-threshold dissociation and rescattering.

Angular correlation between photoelectrons and auger electrons from K-shell ionization of neon.

We have used cold target recoil ion momentum spectroscopy to study the continuum correlation between the photoelectron of core-photoionized neon and the subsequent Auger electron. We observe a strong angular correlation between the two electrons. Classical trajectory Monte Carlo calculations agree quite well with the photoelectron energy distribution that is shifted due to the potential change associated with Auger decay.

Observing the creation of electronic feshbach resonances in soft x-ray-induced O2 dissociation.

When an atom or molecule is ionized by an x-ray, highly excited states can be created that then decay, or autoionize, by ejecting a second electron from the ion. We found that autoionization after soft x-ray photoionization of molecular oxygen follows a complex multistep process. By interrupting the autoionization process with a short laser pulse, we showed that autoionization cannot occur until the internuclear separation of the fragments is greater than approximately 30 angstroms.

Time-resolved momentum imaging system for molecular dynamics studies using a tabletop ultrafast extreme-ultraviolet light source.

We describe a momentum imaging setup for direct time-resolved studies of ionization-induced molecular dynamics. This system uses a tabletop ultrafast extreme-ultraviolet (EUV) light source based on high harmonic upconversion of a femtosecond laser. The high photon energy (around 42 eV) allows access to inner-valence states of a variety of small molecules via single photon excitation, while the sub--10-fs pulse duration makes it possible to follow the resulting dynamics in real time.

Large-angle electron diffraction structure in laser-induced rescattering from rare gases.

We have measured full momentum images of electrons rescattered from Xe, Kr, and Ar following the liberation of the electrons from these atoms by short, intense laser pulses. At high momenta the spectra show angular structure (diffraction) which is very target dependent and in good agreement with calculated differential cross sections for the scattering of free electrons from the corresponding ionic cores.

Interference in the collective electron momentum in double photoionization of H2.

We investigate single-photon double ionization of H(2) by 130 to 240 eV circularly polarized photons. We find a double slitlike interference pattern in the sum momentum of both electrons in the molecular frame which survives integration over all other degrees of freedom. The difference momentum and the individual electron momentum distributions do not show such a robust interference pattern.

The simplest double slit: interference and entanglement in double photoionization of H2.

The wave nature of particles is rarely observed, in part because of their very short de Broglie wavelengths in most situations. However, even with wavelengths close to the size of their surroundings, the particles couple to their environment (for example, by gravity, Coulomb interaction, or thermal radiation). These couplings shift the wave phases, often in an uncontrolled way, and the resulting decoherence, or loss of phase integrity, is thought to be a main cause of the transition from quantum to classical behavior.

Soft X-ray-driven femtosecond molecular dynamics.

The direct observation of molecular dynamics initiated by x-rays has been hindered to date by the lack of bright femtosecond sources of short-wavelength light. We used soft x-ray beams generated by high-harmonic upconversion of a femtosecond laser to photoionize a nitrogen molecule, creating highly excited molecular cations. A strong infrared pulse was then used to probe the ultrafast electronic and nuclear dynamics as the molecule exploded.

Routes to control of H2 Coulomb explosion in few-cycle laser pulses.

We have measured coincident ion pairs produced in the Coulomb explosion of H2 by 8-30 fs laser pulses at different laser intensities. We show how the Coulomb explosion of H2 can be experimentally controlled by tuning the appropriate pulse duration and laser intensity. For laser pulses less than 15 fs, we found that the rescattering-induced Coulomb explosion is dominated by first-return recollisions, while for longer pulses and at the proper laser intensity, the third return can be made to be the major one.

Effects of molecular structure on ion disintegration patterns in ionization of O2 and N2 by short laser pulses.

We demonstrate that the structure of the outermost orbitals of oxygen and nitrogen can be observed in the angular distribution of coincident ion pairs generated by the double ionization of these molecules by 8 fs laser pulses. We do this by establishing that these ions emerge from well defined excited electronic states of O2+2 and N2+2 respectively and that they are produced dominantly through a process which involves electron rescattering. The angular distributions of the ions from the two targets are very different, reflecting the different structures of the outermost orbitals of the two molecules.