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.

Multi-particle momentum correlations extracted using covariance methods on multiple-ionization of diiodomethane molecules by soft-X-ray free-electron laser pulses.

Momenta of ions from diiodomethane molecules after multiple ionization by soft-X-ray free-electron-laser pulses are measured. Correlations between the ion momenta are extracted by covariance methods formulated for the use in multiparticle momentum-resolved ion time-of-flight spectroscopy. Femtosecond dynamics of the dissociating multiply charged diiodomethane cations is discussed and interpreted by using simulations based on a classical Coulomb explosion model including charge evolution.

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 ^{3}P_{0,1,2} and ^{3}D_{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.

Strong-Field Extreme-Ultraviolet Dressing of Atomic Double Excitation.

We report on the experimental observation of a 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 Microjoules. A quantum-mechanical calculation of the time-dependent dipole response of this autoionizing state, driven by classical extreme-ultraviolet (XUV) electric fields, evidences strong-field-induced energy and phase shifts of the doubly excited state, which are extracted from 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 a few meV, induced by strong XUV fields. These results open up a new way of performing nonperturbative XUV nonlinear optics for the light-matter interaction of resonant electronic transitions in atoms at short wavelengths.

Electron spectroscopic study of nanoplasma formation triggered by intense soft x-ray pulses.

Using electron spectroscopy, we investigated the nanoplasma formation process generated in xenon clusters by intense soft x-ray free electron laser (FEL) pulses. We found clear FEL intensity dependence of electron spectra. Multistep ionization and subsequent ionization frustration features are evident for the low FEL-intensity region, and the thermal electron emission emerges at the high FEL intensity. The present FEL intensity dependence of the electron spectra is well addressed by the frustration parameter introduced by Arbeiter and Fennel [New J. Phys. 13, 053022 (2011)].

Complete reconstruction of ultra-broadband isolated attosecond pulses including partial averaging over the angular distribution.

Attosecond streaking is a powerful tool to investigate ultrafast electron dynamics on the attosecond time scale. To obtain the highest temporal resolution in a pump-probe experiment, soft-X-ray (SXR) and infrared (IR) pulses have to be carefully characterized. Here, we present a detailed description of our recent generalization of the Volkov-transform generalized projection algorithm (VTGPA) and its application to multiple overlapping photoelectron bands. This method allows for the complete temporal reconstruction of both IR and SXR pulses under the inclusion of accurate complex photoionization matrix elements (PMEs). In this article, we compare the performance of our new method with traditional algorithms. We particularly focus on the important role played by the photoelectron angular distribution (PAD) which needs to be taken into account for the highest fidelity of attosecond pulse reconstruction. For this purpose, we investigate numerically the influence of the finite collection angle of the electron spectrometer on the retrieval and the obtained pulse parameters. We further theoretically demonstrate the reliability of the reconstruction for pulse durations even shorter than the atomic unit of time.

Using a passively stable attosecond beamline for relative photoemission time delays at high XUV photon energies.

We present and demonstrate an experimental scheme that enables overlap-free reconstruction of attosecond beating by interference of two-photon transitions (RABBITT) measurements at high extreme-ultraviolet (XUV) photon energies. A compact passively-stabilized attosecond beamline employing a multilayer (ML) mirror allows us to obtain XUV pulses consisting of only two odd high-harmonic orders from an attosecond pulse train (APT). We compare our new technique to existing schemes that are used to perform RABBITT measurements and discuss how our scheme resolves the limitations imposed by spectral complexity of the harmonic comb at high photon energies. We further demonstrate first applications of our scheme for rare gases and gas mixtures, and show that this scheme can be extended to gas-molecule mixtures.

Extreme-ultraviolet high-order harmonic generation from few-cycle annular beams.

An annular infrared (IR) laser beam has been used for high-order harmonic generation reaching a cut-off energy of 90 eV for extreme-ultraviolet-infrared (XUV-IR) pump-probe experiments in an intrinsically stable attosecond beamline. The generation of harmonics along the laser axis in the missing portion of the laser beam decreases the IR power load on thin metallic foils that are used for removing the residual IR and shaping the XUV pulses from high-harmonic generation. This finds applications in high-average-power few-cycle laser systems, where high-average IR power destroys the foils. The spatial separation of IR and XUV will, moreover, simplify the realization of attosecond time-resolved measurements.

Photoionization delays in xenon using single-shot referencing in the collinear back-focusing geometry.

Attosecond photoemission delays for all the valence (5p3/2, 5p1/2, 5s, 4d5/2, 4d3/2) subshells of xenon have been accessed using the interferometric RABBITT technique. The 4d subshell delays in Xe have been accessed for the first time, to the best of our knowledge, due to the high photon energy used. A novel technique of single-shot referencing in the collinear back-focusing geometry has been introduced. This enables us to distinguish the signal from principal photoelectron peaks due to ionization by extreme ultraviolet radiation only and infrared-induced sideband contributions, especially in the regions of spectral overlap.

Streaking of 43-attosecond soft-X-ray pulses generated by a passively CEP-stable mid-infrared driver.

Attosecond metrology has so far largely remained limited to titanium:sapphire lasers combined with an active stabilization of the carrier-envelope phase (CEP). These sources limit the achievable photon energy to ∼100 eV which is too low to access X-ray absorption edges of most second- and third-row elements which are central to chemistry, biology and material science. Therefore, intense efforts are underway to extend attosecond metrology to the soft-X-ray (SXR) domain using mid-infrared (mid-IR) drivers. Here, we introduce and experimentally demonstrate a method that solves the long-standing problem of the complete temporal characterization of ultra-broadband (≫10 eV) attosecond pulses. We generalize the recently proposed Volkov-transform generalized projection algorithm (VTGPA) to the case of multiple overlapping photoelectron spectra and demonstrate its application to isolated attosecond pulses. This new approach overcomes all key limitations of previous attosecond-pulse reconstruction methods, in particular the central-momentum approximation (CMA), and it incorporates the physical, complex-valued and energy-dependent photoionization matrix elements. These properties make our approach general and particularly suitable for attosecond supercontinua of arbitrary bandwidth. We apply this method to attosecond SXR pulses generated from a two-cycle mid-IR driver, covering a bandwidth of ∼100 eV and reaching photon energies up to 180 eV. We extract an SXR pulse duration of (43±1) as from our streaking measurements, defining a new world record. Our results prove that the popular and broadly available scheme of post-compressing the output of white-light-seeded optical parametric amplifiers is adequate to produce high-contrast isolated attosecond pulses covering the L-edges of silicon, phosphorous and sulfur. Our new reconstruction method and experimental results open the path to the production and characterization of attosecond pulses lasting less than one atomic unit of time (24 as) and covering X-ray absorption edges of most light elements.

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 an ionized 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.

Photoelectron spectrometer for liquid and gas-phase attosecond spectroscopy with field-free and magnetic bottle operation modes.

A compact time-of-flight spectrometer for applications in attosecond spectroscopy in the liquid and gas phases is presented. It allows for altering the collection efficiency by transitioning between field-free and magnetic-bottle operation modes. High energy resolution (ΔE/E = 0.03 for kinetic energies >20 eV) is achieved despite the short flight-tube length through a homogeneous deceleration potential at the beginning of the flight tube. A closing mechanism allows isolating the vacuum system of the flight tube from the interaction region in order to efficiently perform liquid-microjet experiments. The capabilities of the instrument are demonstrated through photoelectron spectra from multiphoton ionization of argon and xenon, as well as photoelectron spectra of liquid and gaseous water generated by an attosecond pulse train.

Extreme-ultraviolet high-harmonic generation in liquids.

High-harmonic generation (HHG) in gases has been the main enabling technology of attosecond science since its discovery. Recently, HHG from solids has been demonstrated, opening a lively area of research. In contrast, harmonic generation from liquids has so far remained restricted to low harmonics in the visible regime. Here, we report the observation and detailed characterization of extreme ultraviolet HHG from liquid water and several alcohols extending beyond 20 eV. This advance was enabled by the implementation of the recent liquid flat-microjet technology, which we show to facilitate the spatial separation of HHG from the bulk liquid and the surrounding gas phase. We observe striking differences between the HHG spectra of water and several alcohols. A comparison with a strongly-driven few-band model establishes the sensitivity of HHG to the electronic structure of liquids. Our results suggest liquid-phase high-harmonic spectroscopy as a new method for studying the electronic structure and ultrafast scattering processes in liquids.