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

Nonlinear spectroscopy on an autoionizing two-electron resonance in intense, extreme ultraviolet fields at a free-electron laser

In this work, the influence of intense extreme-ultraviolet (XUV) fields on helium is experimentally investigated. Therefore, XUV pulses from a free-electron laser (FEL) are combined with transient absorption spectroscopy (TAS) and explored with numerical quantum-mechanical simulations. A novel TAS beamline enables measurements on the prototypical atomic three-body system, helium, at the free-electron laser in Hamburg (FLASH). In particular, the energetically lowest two-electron resonance, 2s2p, with its asymmetric Fano absorption line shape is of interest. This bound state is embedded in the single-ionization continuum and thus represents an atomic interferometer. Its main property, the sensitivity to phase, is used in this work to detect manipulations induced by strong XUV pulses. In the experiments, a distortion of the absorption line is observed in the presence of highly intense XUV pulses. Firstly, the line shape’s symmetry change is investigated with a numerical few-level model simulation and found to be connected to the transient dressing of the excited state. Employing realistically modelled stochastic pulses, the investigation is extended to the line shape’s dependence on the pulse duration. Finally, the line broadening is explained by the model simulation and allows for disentangling the contributing mechanisms, two-photon absorption and the increased reversion to the ground state

Pulse length effects on autoionizing states under the influence of intense SASE XUV fields

The Fano absorption line shape of an autoionizing state encodes information on its internal atomic structure and dynamics.When driven near-resonantly with intense extreme ultraviolet (XUV) electric fields, the absorption profile can be deliberately modified, including observable changes of both the line-shape asymmetry and strength of the resonance, revealing information on the underlying dynamics of the system in response to such external driving. We report on the influence of the XUV pulse parameters at high intensity that can be achieved with a free-electron laser (FEL) with statistically broadened spectra based on self-amplified spontaneous emission (SASE). More specifically, the impact of the FEL pulse duration is studied for the example of the doubly excited 2s2p resonance in helium, where line-shape modifications have been measured with XUV transient absorption spectroscopy in Fraunhofer-type transmission geometry. A computational few-level-model provides insight into the impact of different average pulse durations of the stochastic FEL pulses. These findings are supported by measurements performed at the Free-Electron Laser in Hamburg (FLASH) and provide further insight into XUV strong-coupling dynamics of resonant transitions driven by intense high-frequency FEL sources

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

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

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

Nonlinear Coherence Effects in Transient-Absorption Ion Spectroscopy with Stochastic Extreme-Ultraviolet Free-Electron Laser Pulses

We demonstrate time-resolved nonlinear extreme-ultraviolet absorption spectroscopy on multiply charged ions, here applied to the doubly charged neon ion, driven by a phase-locked sequence of two intense free-electron laser pulses. Absorption signatures of resonance lines due to $2p-3d$ bound–bound transitions between the spin-orbit multiplets $^3P_{0,1,2}$ and $^3D_{1,2,3}$ of the transiently produced doubly charged Ne$^{2+}$ ion are revealed, with time-dependent spectral changes over a time-delay range of (2.4±0.3) fs. Furthermore, we observe 10-meV-scale spectral shifts of these resonances owing to the ac Stark effect. We use a time-dependent quantum model to explain the observations by an enhanced coupling of the ionic quantum states with the partially coherent free-electron laser radiation when the phase-locked pump and probe pulses precisely overlap in time