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Nature Communications 12(1), 643 (1-7) (2021). doi:10.1038/s41467-020-20846-1, 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., Published by Nature Publishing Group UK, [London]

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., Faraday Discussions, 228, ISSN:1359-6640, ISSN:1364-5498

The femtosecond-timescale formation of a Fano resonance in doubly excited helium has been recently observed, enabling a time-domain view into two-electron correlation dynamics. Measuring the absorption spectral line shape, the buildup of the resonance is revealed by imposing a temporal gate on the dipole response using strong-field ionization. Here, we apply this approach to the Rydberg series of the doubly excited states in helium. This reveals the characteristic times of emergence of isolated two-electron resonances from the continuous single-ionization background absorption, as well as their time-dependent line-shape asymmetry and the time it takes to separate individual spectral absorption lines within the series. Furthermore, we time resolve the dynamics of the excited wave packet by reconstructing its dipole response in the time domain and thereby characterize the ionization gate to close as fast as only 1.2 fs. These results represent an approach to resolve on the femtosecond and attosecond timescale the strong-field-ionization dynamics of excited coherent wave packets.

We present a technique for the direct measurement of the frequency chirp of high-frequency free-electron-laser pulses based on fundamental nonlinear optics. It is implemented in transient absorption geometry.

Accessing attosecond (as) dynamics directly in the time domain has been achieved by several pioneering experiments over the course of the last decade. Extreme ultraviolet (XUV) group delays and, later, ionization time delays on the order of a few attoseconds have been extracted by photoemission or high-harmonic spectroscopy. Here, we present and benchmark an approach based on attosecond transient absorption spectroscopy to quantify deliberately induced delays by employing resonant photoexcitation of three XUV transitions with a precision of less than 5 as. While here we quantify the sensitivity to these delays via a chirp on the attosecond pulse by using thin-foil metallic filters, the method enables future studies of attosecond delays probed through resonant excitations.

We report on the experimental observation of strong-field dressing of an autoionizing two-electron state in helium with intense extreme-ultraviolet laser pulses from a free-electron laser. The asymmetric Fano line shape of this transition is spectrally resolved, and we observe modifications of the resonance asymmetry structure for increasing free-electron-laser pulse energy on the order of few tens of $\mu$J. A quantum-mechanical calculation of the time-dependent dipole response of this autoionizing state, driven by classical extreme-ultraviolet (XUV) electric fields, reveals a direct link between strong-field-induced energy and phase shifts of the doubly excited state and the Fano line-shape asymmetry. The experimental results obtained at the Free-Electron Laser in Hamburg (FLASH) thus correspond to transient energy shifts on the order of few meV, induced by strong XUV fields. These results open up a new way of performing non-perturbative XUV nonlinear optics for the light-matter interaction of resonant electronic transitions in atoms at short wavelengths., Comment: 16 pages, 3 figures

Measuring bound-state quantum dynamics, excited and driven by strong fields, is achievable by time-resolved absorption spectroscopy. Here, a vacuum beamline for spectroscopy in the attosecond temporal and extreme ultraviolet (XUV) spectral range is presented, which is a tool for observing and controlling nonequilibrium electron dynamics. In particular, we introduce a technique to record an XUV absorption signal and the corresponding reference simultaneously, which greatly improves the signal quality. The apparatus is based on a common beam path design for XUV and near-infrared (NIR) laser light in a vacuum. This ensures minimal spatiotemporal fluctuations between the strong NIR laser and the XUV excitation and reference beams, while the grazing incidence optics enable broadband spectral coverage. The apparatus combines high spectral and temporal resolution together with an increase in sensitivity to weak absorption signatures by an order of magnitude. This opens up new possibilities for studying strong-field-driven electron dynamics in bound systems on their natural attosecond time scale.

The laser-field-modified dipole response of the first ionization threshold of helium is studied by means of attosecond transient absorption spectroscopy. We resolve light-induced time-dependent structures in the photoabsorption spectrum both below and above the ionization threshold. By comparing the measured results to a quantum-dynamical model, we isolate the contributions of the unbound electron to these structures. They originate from light-induced couplings of near-threshold bound and continuum states and light-induced energy shifts of the free electron. The ponderomotive energy, at low laser intensities, is identified as a good approximation for the perturbed continuum response.

Physical review letters 123(10), 103001 (2019). doi:10.1103/PhysRevLett.123.103001, 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., Published by APS, College Park, Md.