UV 30†fs laser pulse generation using a multi-pass cell.

Ultrashort ultraviolet (UV) pulses are pivotal for resolving ultrafast electron dynamics. However, their efficient generation is strongly impeded by material dispersion and two-photon absorption, in particular, if pulse durations around a few tens of femtoseconds or below are targeted. Here, we present a new (to our knowledge) approach to ultrashort UV pulse generation: using the fourth-harmonic generation output of a commercial ytterbium laser system delivering 220 fs UV pulses, we implement a multi-pass cell (MPC) providing 5.6 µJ pulses at 256 nm, compressed to 30.5 fs. Our results set a short-wavelength record for MPC post-compression while offering attractive options to navigate the trade-off between upconversion efficiency and acceptance bandwidth for UV pulse production.

Deriving x-ray pulse duration from center-of-energy shifts in THz-streaked ionized electron spectra.

A fast and robust, yet simple, method has been developed for the immediate characterization of x-ray pulse durations via IR/THz streaking that uses the center of energy (COE) of the photoelectron spectrum for the evaluation. The manuscript presents theory and numerical models demonstrating that the maximum COEs shift as a function of the pulse duration and compares them to existing data for validation. It further establishes that the maximum COE can be derived from two COE measurements set at a phase of π/2 apart. The theory, model, and data agree with each other very well, and they present a way to measure pulse durations ranging from sub-fs to tens of fs on-the-fly with a fairly simple experimental setup.

Ultrafast electron cooling in an expanding ultracold plasma.

Plasma dynamics critically depends on density and temperature, thus well-controlled experimental realizations are essential benchmarks for theoretical models. The formation of an ultracold plasma can be triggered by ionizing a tunable number of atoms in a micrometer-sized volume of a 87Rb Bose-Einstein condensate (BEC) by a single femtosecond laser pulse. The large density combined with the low temperature of the BEC give rise to an initially strongly coupled plasma in a so far unexplored regime bridging ultracold neutral plasma and ionized nanoclusters. Here, we report on ultrafast cooling of electrons, trapped on orbital trajectories in the long-range Coulomb potential of the dense ionic core, with a cooling rate of 400 K ps-1. Furthermore, our experimental setup grants direct access to the electron temperature that relaxes from 5250 K to below 10 K in less than 500 ns.

THz streak camera performance for single-shot characterization of XUV pulses with complex temporal structures.

The THz-field-driven streak camera has proven to be a powerful diagnostic-technique that enables the shot-to-shot characterization of the duration and the arrival time jitter of free electron laser (FEL) pulses. Here we investigate the performance of three computational approaches capable to determine the duration of FEL pulses with complex temporal structures from single-shot measurements of up to three simultaneously recorded spectra. We use numerically simulated FEL pulses in order to validate the accuracy of the pulse length retrieval in average as well as in a single-shot mode. We discuss requirements for the THz field strength in order to achieve reliable results and compare our numerical study with the analysis of experimental data that were obtained at the FEL in Hamburg - FLASH.

Time-Resolved Dissociation Dynamics of Iodomethane Resulting from Rydberg and Valence Excitation.

Rydberg excitations in the vacuum ultraviolet spectral range may open up molecular photoreaction pathways not accessible from lower-lying valence states. Here, single-shot UV/VUV pump-probe spectroscopy was used to study the photodissociation dynamics of iodomethane after 268 nm excitation in the A-band and excitation of the 6p (2 E3/2) Rydberg state at 161 nm. By combining weak-field VUV single-photon ionization with sub-10 fs temporal resolution and the superior statistical accuracy of the single-shot technique, sub-30 fs wave packet dynamics upon excitation in the A-band by a UV pump pulse were disclosed. Population transfer from the Rydberg state to the 2 1 A1 valence state leading to 100 fs dissociation dynamics was observed by utilizing the same methodology in a VUV-pump/UV-probe scheme.

Correlated electronic decay in expanding clusters triggered by intense XUV pulses from a Free-Electron-Laser.

Irradiation of nanoscale clusters and large molecules with intense laser pulses transforms them into highly-excited non- equilibrium states. The dynamics of intense laser-cluster interaction is encoded in electron kinetic energy spectra, which contain signatures of direct photoelectron emission as well as emission of thermalized nanoplasma electrons. In this work we report on a so far not observed spectrally narrow bound state signature in the electron kinetic energy spectra from mixed Xe core - Ar shell clusters ionized by intense extreme-ultraviolet (XUV) pulses from a free-electron-laser. This signature is attributed to the correlated electronic decay (CED) process, in which an excited atom relaxes and the excess energy is used to ionize the same or another excited atom or a nanoplasma electron. By applying the terahertz field streaking principle we demonstrate that CED-electrons are emitted at least a few picoseconds after the ionizing XUV pulse has ended. Following the recent finding of CED in clusters ionized by intense near-infrared laser pulses, our observation of CED in the XUV range suggests that this process is of general relevance for the relaxation dynamics in laser produced nanoplasmas.

Direct observation of isolated Damon-Eshbach and backward volume spin-wave packets in ferromagnetic microstripes.

The analysis of isolated spin-wave packets is crucial for the understanding of magnetic transport phenomena and is particularly interesting for applications in spintronic and magnonic devices, where isolated spin-wave packets implement an information processing scheme with negligible residual heat loss. We have captured microscale magnetization dynamics of single spin-wave packets in metallic ferromagnets in space and time. Using an optically driven high-current picosecond pulse source in combination with time-resolved scanning Kerr microscopy probed by femtosecond laser pulses, we demonstrate phase-sensitive real-space observation of spin-wave packets in confined permalloy (Ni80Fe20) microstripes. Impulsive excitation permits extraction of the dynamical parameters, i.e. phase- and group velocities, frequencies and wave vectors. In addition to well-established Damon-Eshbach modes our study reveals waves with counterpropagating group- and phase-velocities. Such unusual spin-wave motion is expected for backward volume modes where the phase fronts approach the excitation volume rather than emerging out of it due to the negative slope of the dispersion relation. These modes are difficult to excite and observe directly but feature analogies to negative refractive index materials, thus enabling model studies of wave propagation inside metamaterials.

Efficient generation of below-threshold harmonics for high-fidelity multi-photon physics in the VUV spectral range.

We demonstrate the generation of microjoule level, sub-20-fs, Ti:Sa fifth-harmonic pulses utilizing a loose-focusing geometry in a long Ar gas cell. The VUV pulses centered at 161.8 nm reach pulse energies of 1.1 µJ per pulse, while the corresponding pulse duration is measured with a second-order, fringe-resolved autocorrelation scheme to be 18±1 fs. Nonresonant, two-photon ionization of Kr and three-photon ionization of Ne verify the fifth-harmonic pulse high-intensity content and indicate the feasibility of multi-photon VUV pump-VUV probe studies of ultrafast atomic and molecular dynamics.

Electron wave packet sampling with laser-generated extreme ultraviolet and terahertz fields.

We report on transferring the concept of light-field streaking with intense terahertz fields from free-electron lasers to the laboratory scale. Utilizing a commercial laser system, synchronized 300 µm terahertz and 13 nm extreme ultraviolet pulses are generated by optical rectification and high harmonic generation, respectively. The terahertz fields are sufficiently strong to support electron wave packet sampling with a few fs resolution. The capability of this approach is demonstrated by measuring the duration of electron pulses formed by direct photoemission from a neon gas target.

Ultrafast photofragmentation dynamics of molecular iodine driven with timed XUV and near-infrared light pulses.

Photofragmentation dynamics of molecular iodine was studied as a response to the joint illumination with femtosecond 800 nm near-infrared and 13 nm extreme ultraviolet (XUV) pulses delivered by the free-electron laser facility FLASH. The interaction of the molecular target with two light pulses of different wavelengths but comparable pulse energy elucidates a complex intertwined electronic and nuclear dynamics. To follow distinct pathways out of a multitude of reaction channels, the recoil of created ionic fragments is analyzed. The delayed XUV pulse provides a way of following molecular photodissociation of I(2) with a characteristic time-constant of (55 ± 10) fs after the laser-induced formation of antibonding states. A preceding XUV pulse, on the other hand, preferably creates a 4d(-1) inner-shell vacancy followed by the fast Auger cascade with a revealed characteristic time constant τ(A2)=(23±11) fs for the second Auger decay transition. Some fraction of molecular cationic states undergoes subsequent Coulomb explosion, and the evolution of the launched molecular wave packet on the repulsive Coulomb potential was accessed by the laser-induced postionization. A further unexpected photofragmentation channel, which relies on the collective action of XUV and laser fields, is attributed to a laser-promoted charge transfer transition in the exploding molecule.

Time resolved Fano resonances.

Recent advances in the generation of sub-fs extreme ultraviolet pulses and attosecond metrology have opened up the possibility to trace the time evolution of electronic wave packets inside atoms in pump-probe experiments. We investigate the feasibility of observing the buildup of a Fano resonance in the time domain by attosecond streaking techniques. A time-resolved resonance is initialized by a sub-fs extreme ultraviolet-pump pulse in the presence of a synchronized phase-controlled probe laser pulse. The time evolution of the coherent superposition of resonant state and continuum is mapped onto a modulation of the electron spectrum as a function of the time delay between pump and probe pulse. (super-)Coster-Kronig transitions with lifetimes of approximately 400 asec( are identified as prime candidates.