Flexible experimental platform for dispersion-free temporal characterization of ultrashort pulses

The precise temporal characterization of laser pulses is crucial for ultrashort applications in biology, chemistry, and physics. Especially in femto- and attosecond science, diverse laser pulse sources in different spectral regimes from the visible to the short-wavelength infrared as well as pulse durations ranging from picoseconds to few femtoseconds are employed. In this article, we present a versatile temporal-characterization apparatus that can access these different temporal and spectral regions in a dispersion-free manner and without phase-matching constraints. The design combines transient-grating and surface third-harmonic-generation frequency-resolved optical gating in one device with optimized alignment capabilities based on a noncollinear geometry

Time-and-Energy–Resolved Electron Dynamics in Atoms and Molecules with Intense Short-Wavelength Light

This thesis investigates the interaction of ultrashort, extreme-ultraviolet (XUV) and soft x-ray laser pulses with atoms and molecules in the gas phase. In total, the subject is explored from four different perspectives, which are all based on the short- lived–coherent electronic responses to the laser pulses, and measured with transient absorption spectroscopy. First, a theoretical study reveals how transient energy shifts of electronic dressed states in atoms driven by an intense XUV Free-Electron Laser (FEL) lead to temporal dipole phase shifts and absorption-line changes. Second, a follow-up study investigates the electronic-population Rabi-cycles corresponding to the absorption-line changes of the first study. A convolutional neural network is employed to reconstruct the temporal population dynamics from the simulated spectral absorption modifications. The inversion from an absorption to an emission line is described and a potential experimental demonstration in helium is discussed. Third, dense gas targets enable amplification of the otherwise improbable, non-linear process of stimulated resonant inelastic x-ray scattering (RIXS), as well as x-ray FEL propagation-based spatial-spectral reshaping. To this end, a new experimental setup is built and utilized in an x-ray FEL driven RIXS experiment in dense neon gas. Fourth, a novel experiment combining XUV pulses from high-order harmonic generation (HHG) and XUV-FEL pulses is demonstrated by time-resolving a photochemical reaction in molecular oxygen. An FEL pulse initiates coupled nuclear-electronic dissociation pathways from molecular oxygen ions, which are time-resolved on femto- and picosecond time scales by identifying the reaction products in the time-delayed HHG absorption spectra. A FEL-photon-energy–resolved study of the fragments is performed to compare findings from absorption spectroscopy with kinetic energy release spectra recorded in parallel with a reaction microscope

Elektronen-Korrelation in Helium unter Einfluss intensiver XUV-Laserpulse

In this work the interaction of helium with intensive XUV-pulses is investigated numerically to interpret the experiments (june 2016) performed at FLASH (Free-Electron-Laser in Hamburg). For this purpose the helium atom can be regarded as a few-level-model, furthermore the electron-correlation as well as the coupling with the continuum are considered. The time-dependent Schrödinger equation of the system is solved with discrete time steps. The result is an intensity dependent variation of the observed 2s2p resonance's line shape. This variation is explained by an energy-change induced phase-shift. With this, results and explanations of similar experiments using intense IR-pulses and weak high harmonics can be conrmed. First steps of the inuence on this line shape variation due to noisy XUV-pulses produced at FLASH are investigated as well

Electronic Population Reconstruction from Strong-Field-Modified Absorption Spectra with a Convolutional Neural Network

We simulate ultrafast electronic transitions in an atom and corresponding absorption line changes with a numerical, few-level model, similar to previous work. In addition, a convolutional neural network (CNN) is employed for the first time to predict electronic state populations based on the simulated modifications of the absorption lines. We utilize a two-level and four-level system, as well as a variety of laser-pulse peak intensities and detunings, to account for different common scenarios of light–matter interaction. As a first step towards the use of CNNs for experimental absorption data in the future, we apply two different noise levels to the simulated input absorption data

Differential Measurement of Electron Ejection after Two-Photon Two-Electron Excitation of Helium

We report the measurement of the photoelectron angular distribution of two-photon single-ionization near the $2p^2$ $^1D^e$ double-excitation resonance in helium, benchmarking the fundamental nonlinear interaction of two photons with two correlated electrons. This observation is enabled by the unique combination of intense extreme ultraviolet pulses, delivered at the high-repetition-rate free-electron laser in Hamburg (FLASH), ionizing a jet of cryogenically cooled helium atoms in a reaction microscope. The spectral structure of the intense self-amplified spontaneous emission free-electron laser pulses has been resolved on a single-shot level to allow for post selection of pulses, leading to an enhanced spectral resolution, and introducing a new experimental method. The measured angular distribution is directly compared to state-of-the-art theory based on multichannel quantum defect theory and the streamlined $R$-matrix method. These results and experimental methodology open a promising route for exploring fundamental interactions of few photons with few electrons in general

XUV pump-XUV probe transient absorption spectroscopy at FELs

The emergence of ultra-intense extreme-ultraviolet (XUV) and X-ray free-electron lasers (FELs) has opened the door for the experimental realization of non-linear XUV and X-ray spectroscopy techniques. Here we demonstrate an experimental setup for an all-XUV transient absorption spectroscopy method for gas-phase targets at the FEL. The setup combines a high spectral resolving power of E/ΔE ≈ 1500 with sub-femtosecond interferometric resolution, and covers a broad XUV photon-energy range between approximately 20 and 110 eV. We demonstrate the feasibility of this setup firstly on a neon target. Here, we intensity- and time-resolve key aspects of non-linear XUV-FEL light-matter interactions, namely the non-resonant ionization dynamics and resonant coupling dynamics of bound states, including XUV-induced Stark shifts of energy levels. Secondly, we show that this setup is capable of tracking the XUV-initiated dissociation dynamics of small molecular targets (oxygen and diiodomethane) with site-specific resolution, by measuring the XUV transient absorption spectrum. In general, benefitting from a single-shot detection capability, we show that the setup and method provides single-shot phase-locked XUV pulse pairs. This lays the foundation to perform, in the future, experiments as a function of the XUV interferometric time delay and the relative phase, which enables advanced coherent non-linear spectroscopy schemes in the XUV and X-ray spectral range.ISSN:1359-6640ISSN:1364-549

XUV pump–XUV probe transient absorption spectroscopy at FELs

The emergence of ultra-intense extreme-ultraviolet (XUV) and X-ray free-electron lasers (FELs) has opened the door for the experimental realization of non-linear XUV and X-ray spectroscopy techniques. Here we demonstrate an experimental setup for an all-XUV transient absorption spectroscopy method for gas-phase targets at the FEL. The setup combines a high spectral resolving power of $E/ΔE$ ≈ 1500 with sub-femtosecond interferometric resolution, and covers a broad XUV photon-energy range between approximately 20 and 110 eV. We demonstrate the feasibility of this setup firstly on a neon target. Here, we intensity- and time-resolve key aspects of non-linear XUV-FEL light–matter interactions, namely the non-resonant ionization dynamics and resonant coupling dynamics of bound states, including XUV-induced Stark shifts of energy levels. Secondly, we show that this setup is capable of tracking the XUV-initiated dissociation dynamics of small molecular targets (oxygen and diiodomethane) with site-specific resolution, by measuring the XUV transient absorption spectrum. In general, benefitting from a single-shot detection capability, we show that the setup and method provides single-shot phase-locked XUV pulse pairs. This lays the foundation to perform, in the future, experiments as a function of the XUV interferometric time delay and the relative phase, which enables advanced coherent non-linear spectroscopy schemes in the XUV and X-ray spectral range

XUV-Initiated Dissociation Dynamics of Molecular Oxygen (O2_2)

We performed a time-resolved spectroscopy experixment on the dissociation of oxygen molecules after the interactionwith intense extreme-ultraviolet (XUV) light from the free-electronlaser in Hamburg at Deutsches Elektronen-Synchrotron. Using anXUV-pump/XUV-probe transient-absorption geometry with asplit-and-delay unit, we observe the onset of electronic transitionsin the O$^{2+}$ cation near 50 eV photon energy, marking the end ofthe progression from a molecule to two isolated atoms. We observetwo different time scales of 290 ± 53 and 180 ± 76 fs for theemergence of different ionic transitions, indicating differentdissociation pathways taken by the departing oxygen atoms.With regard to the emerging opportunities of tuning the centralfrequencies of pump and probe pulses and of increasing the probe−pulse bandwidth, future pump−probe transient-absorptionexperiments are expected to provide a detailed view of the coupled nuclear and electronic dynamics during molecular dissociatio

Measuring the frequency chirp of extreme-ultraviolet free-electron laser pulses by transient absorption spectroscopy

High-intensity ultrashort pulses at extreme ultraviolet (XUV) and x-ray photon energies, delivered by state-of-the-art free-electron lasers (FELs), are revolutionizing the field of ultrafast spectroscopy. For crossing the next frontiers of research, precise, reliable and practical photonic tools for the spectro-temporal characterization of the pulses are becoming steadily more important. Here, we experimentally demonstrate a technique for the direct measurement of the frequency chirp of extreme-ultraviolet free-electron laser pulses based on fundamental nonlinear optics. It is implemented in XUV-only pump-probe transient-absorption geometry and provides in-situ information on the time-energy structure of FEL pulses. Using a rate-equation model for the time-dependent absorbance changes of anionized neon target, we show how the frequency chirp can be directly extracted and quantified from measured data. Since the method does not rely on an additional external field, we expect a widespread implementation at FELs benefiting multiple science fields by in-situ on-target measurement and optimization of FEL-pulse properties

Strong-Field Extreme-Ultraviolet Dressing of Atomic Double Excitation

We report on the experimental observation of a strong-field dressing of an autoionizing two-electronstate in helium with intense extreme-ultraviolet laser pulses from a free-electron laser. The asymmetricFano line shape of this transition is spectrally resolved, and we observe modifications of the resonanceasymmetry structure for increasing free-electron-laser pulse energy on the order of few tens of Microjoules.A quantum-mechanical calculation of the time-dependent dipole response of this autoionizing state, drivenby classical extreme-ultraviolet (XUV) electric fields, evidences strong-field-induced energy and phaseshifts of the doubly excited state, which are extracted from the Fano line-shape asymmetry. Theexperimental results obtained at the Free-Electron Laser in Hamburg (FLASH) thus correspond to transientenergy shifts on the order of a few meV, induced by strong XUV fields. These results open up a new way ofperforming nonperturbative XUV nonlinear optics for the light-matter interaction of resonant electronictransitions in atoms at short wavelengths