Extreme Ultraviolet Pulses Research Articles

Compact realization of all-attosecond pump-probe spectroscopy.

The ability to perform attosecond-pump attosecond-probe spectroscopy (APAPS) is a longstanding goal in ultrafast science. While first pioneering experiments demonstrated the feasibility of APAPS, the low repetition rates (10 to 120 Hz) and the large footprints of existing setups have so far hindered the widespread exploitation of APAPS. Here, we demonstrate two-color APAPS using a commercial laser system at 1 kHz, straightforward post-compression in a hollow-core fiber, and a compact high-harmonic generation (HHG) setup. The latter enables the generation of intense extreme-ultraviolet (XUV) pulses by using an out-of-focus HHG geometry and by exploiting a transient blueshift of the driving laser in the HHG medium. Near-isolated attosecond pulses are generated, as demonstrated by one-color and two-color XUV-pump XUV-probe experiments. Our concept allows selective pumping and probing on extremely short timescales in many laboratories and permits investigations of fundamental processes that are not accessible by other pump-probe techniques.

Attosecond-pump attosecond-probe x-ray spectroscopy of liquid water.

Attosecond-pump/attosecond-probe experiments have long been sought as the most straightforward method for observing electron dynamics in real time. Although there has been much success with overlapped near-infrared femtosecond and extreme ultraviolet attosecond pulses combined with theory, true attosecond-pump/attosecond-probe experiments have been limited. We used a synchronized attosecond x-ray pulse pair from an x-ray free-electron laser to study the electronic response to valence ionization in liquid water through all x-ray attosecond transient absorption spectroscopy (AX-ATAS). Our analysis showed that the AX-ATAS response is confined to the subfemtosecond timescale, eliminating any hydrogen atom motion and demonstrating experimentally that the 1b1 splitting in the x-ray emission spectrum is related to dynamics and is not evidence of two structural motifs in ambient liquid water.

Dissociation and Isomerization Following Ionization of Ethylene: Insights from Nonadiabatic Dynamics Simulations.

Photoionized and electronically excited ethylene C2H4+ can undergo H-loss, H2-loss, and ethylene-ethylidene isomerization, where the latter entails a hydrogen migration. Recent pioneering experiments with few-femtosecond extreme ultraviolet pulses and complementary theoretical studies have shed light on the photodynamics of this prototypical organic cation. However, no theoretical investigation based on dynamics simulations reported to date has described the mechanisms and time scales of dissociation and isomerization. Herein, we simulate the coupled electron-nuclear dynamics of ethylene following vertical ionization and electronic excitation to its four lowest-lying cationic states. The electronic structure is treated at the CASSCF level, with an active space large enough to describe bond breaking and formation. The simulations indicate that dissociation and isomerization take place mainly on the cationic ground state and allow the probing of previous hypotheses concerning the correlation between the photochemical outcome and the traversed conical intersections. The results, moreover, support the long-standing view that H2-loss may occur from the ethylidene form. However, the ethylene-ethylidene isomerization time predicted by the simulations is considerably longer than those previously inferred from indirect experimental measurements.

Shaping extreme-ultraviolet attosecond pulses by tuning the minimum in high-order harmonic generation with two gas jets

Shaping extreme-ultraviolet attosecond pulses by tuning the minimum in high-order harmonic generation with two gas jets

Extreme ultraviolet time-resolved photoelectron spectroscopy of adenine, adenosine and adenosine monophosphate in a liquid flat jet.

Time-resolved photoelectron spectroscopy using an extreme-ultraviolet (XUV) probe pulse was used to investigate the UV photoinduced dynamics of adenine (Ade), adenosine (Ado), and adenosine-5-monophosphate (AMP) in a liquid water jet. In contrast to previous studies using UV probe pulses, the XUV pulse at 21.7 eV can photoionize all excited states of a molecule, allowing for full relaxation pathways to be addressed after excitation at 4.66 eV. This work was carried out using a gas-dynamic flat liquid jet, resulting in considerably enhanced signal compared to a cylindrical jet. All three species decay on multiple time scales that are assigned based on their decay associated spectra; the fastest decay of ∼100 fs is assigned to ππ* decay to the ground state, while a smaller component with a lifetime of ∼500 fs is attributed to the nπ* state. An additional slower channel in Ade is assigned to the 7H Ade conformer, as seen previously. This work demonstrates the capability of XUV-TRPES to disentangle non-adiabatic dynamics in an aqueous solution in a state-specific manner and represents the first identification of the nπ* state in the relaxation dynamics of adenine and its derivatives.

Control of Ion-Photoelectron Entanglement and Coherence Via Rabi Oscillations.

We report a theoretical investigation of photoionization by a pair of coherent, ultrashort, fundamental and second-harmonic extreme-ultraviolet pulses, where the photon energies are selected to yield the same photoelectron energy for ionization of two different subshells. This choice implies that the fundamental energy is equal to the difference in energy of the ionic states and that they are therefore coupled by the fundamental photon. By deriving analytical expressions using the essential-states approach, we show that this Rabi coupling creates coherence between the two photoelectron wave packets, which would otherwise be incoherent. We analyze how the coupling is affected by the parameters, such as relative phase, pulse width, delay between the two pulses, Rabi coupling strength, and photoelectron energy. Our discussion mostly considers Ne 2p and 2s photoionization, but it is generally valid for many other quantum systems where photoionization from two different shells is observed.

XUV Rectification Effect in the IR-Dressed Medium.

We show that the quasistatic dipole moment can be induced by a short extreme ultraviolet (XUV) pulse (XUV rectification effect) in atomic gas medium subjected to an intense infrared (IR) field (IR-dressed atoms). The general theory of the XUV rectification effect for a single IR-dressed atom is presented, which explicitly relates IR-modified polarizability of an atomic system in the XUV range with the induced quasistatic dipole moment. We illustrate general properties of the XUV rectification effect in an atomic system within the analytical zero-range potential model by presenting the dependence on the IR-field intensity and the time delay between XUV and IR pulses.

Time‐Resolved Photoemission Electron Microscopy on a ZnO Surface Using an Extreme Ultraviolet Attosecond Pulse Pair

AbstractElectrons photoemitted by extreme ultraviolet attosecond pulses derive spatially from the first few atomic surface layers and energetically from the valence band and highest atomic orbitals. As a result, it is possible to probe the emission dynamics from a narrow 2D region in the presence of optical fields, as well as obtain elemental specific information. However, combining this with spatially‐resolved imaging is a long‐standing challenge because of the large inherent spectral width of attosecond pulses, as well as the difficulty of making them at high repetition rates. Here, this work demonstrates an attosecond interferometry experiment on a zinc oxide (ZnO) surface using spatially and energetically resolved photoelectrons. Photoemission electron microscopy is combined with near‐infrared pump ‐ extreme ultraviolet probe laser spectroscopy and the instantaneous phase of an infrared field is resolved with high spatial resolution. Results show how the core level states with low binding energy of ZnO are well suited to perform spatially resolved attosecond interferometry experiments. A distinct phase shift of the attosecond beat signal is observed across the laser focus which is attributed to wavefront differences between the pump and the probe fields at the surface. This work demonstrates a clear pathway for attosecond interferometry with high spatial resolution at atomic scale surface regions opening up for a detailed understanding of nanometric light‐matter interaction.

Time-resolving state-specific molecular dissociation with XUV broadband absorption spectroscopy.

The electronic and nuclear dynamics inside molecules are essential for chemical reactions, where different pathways typically unfold on ultrafast timescales. Extreme ultraviolet (XUV) light pulses generated by free-electron lasers (FELs) allow atomic-site and electronic-state selectivity, triggering specific molecular dynamics while providing femtosecond resolution. Yet, time-resolved experiments are either blind to neutral fragments or limited by the spectral bandwidth of FEL pulses. Here, we combine a broadband XUV probe pulse from high-order harmonic generation with an FEL pump pulse to observe dissociation pathways leading to fragments in different quantum states. We temporally resolve the dissociation of a specific O2+ state into two competing channels by measuring the resonances of ionic and neutral fragments. This scheme can be applied to investigate convoluted dynamics in larger molecules relevant to diverse science fields.

Electron vortices generation of photoelectron of H2+ by counter-rotating circularly polarized attosecond pulses

Molecular-frame photoelectron momentum distributions (MF-PMDs) of an H2+ molecule ion in the presence of a pair of counter-rotating circularly polarized attosecond extreme ultraviolet laser pulses is studied by numerically solving the two-dimensional time-dependent Schrödinger equation within the frozen-nuclei approximation. At small time delay, our simulations show that the electron vortex structure is sensitive to the time delay and relative phase between the counter-rotating pulses when they are partially overlapped. By adjusting time delay and relative phase, we have the ability to manipulate the MF-PMDs and the appearance of spiral arms. We further show that the internuclear distance can affect the spiral vortices due to its different transition cross sections in the parallel and perpendicular geometries. The lowest-order perturbation theory is employed to interpret these phenomena qualitatively. It is concluded that the internuclear distance-dependent transition cross sections and the confinement effect in diatomic molecules are responsible for the variation of vortex structures in the MF-PMDs.

Atom probe tomography using an extreme ultraviolet trigger pulse.

Atom probe tomography (APT) is a powerful materials characterization technique capable of measuring the isotopically resolved three-dimensional (3D) structure of nanoscale specimens with atomic resolution. Modern APT instrumentation most often uses an optical pulse to trigger field ion evaporation-most commonly, the second or third harmonic of a Nd laser is utilized (∼λ = 532 nm or λ = 355 nm). Herein, we describe an APT instrument that utilizes ultrafast extreme ultraviolet (EUV) optical pulses to trigger field ion emission. The EUV light is generated via a commercially available high harmonic generation system based on a noble-gas-filled capillary. The centroid of the EUV spectrum is tunable from around 25eV (λ = 50 nm) to 45eV (λ = 28 nm), dependent on the identity of the gas in the capillary (Xe, Kr, or Ar). EUV pulses are delivered to the APT analysis chamber via a vacuum beamline that was optimized to maximize photon flux at the APT specimen apex while minimizing complexity. We describe the design of the beamline in detail, including the various compromises involved. We characterize the spectrum of the EUV light and its evolution as it propagates through the various optical elements. The EUV focus spot size is measured at the APT specimen plane, and the effects of misalignment are simulated and discussed. The long-term stability of the EUV source has been demonstrated for more than a year. Finally, APT mass spectra are shown, demonstrating the instrument's ability to successfully trigger field ion emission from semiconductors (Si, GaN) and insulating materials (Al2O3).

Imaging and Controlling Ultrafast Electron Pulses Emitted from Plasmonic Nanostructures.

We experimentally study photoemission from gold nanodisk arrays using space-, time-, and energy-resolved photoemission electron microscopy. When excited by a plasmonic resonant infrared (IR) laser pulse, plasmonic hotspots are generated owing to local surface plasmon resonance. Photoelectrons emitted from each plasmonic hotspot form a nanoscale and ultrashort electron pulse. When the system is excited by an extreme ultraviolet (EUV) laser pulse, a uniformly distributed photoelectron cloud is formed across the sample surface. When excited by the IR and EUV laser pulses together, both the photoemission image and kinetic energy vary significantly for the IR laser-generated electrons depending on the time delay between the two laser pulses. These observations are well explained by the Coulomb interaction with the EUV laser-generated electron cloud. Our study offers a feasible approach to manipulate the energy of electron pulse emitted from a plasmonic nanostructure on an ultrafast time scale.

Three-dimensional coherent diffraction snapshot imaging using extreme-ultraviolet radiation from a free electron laser

The possibility of obtaining a three-dimensional (3D) representation of a single object with sub-µm resolution is crucial in many fields, from material science to clinical diagnostics. This is typically achieved through tomography, which combines multiple 2D images of the same object captured with different orientations. However, this serial imaging method prevents single-shot acquisition in imaging experiments, a mandatory feature for the development of time-resolved 3D imaging. In the present experiment, we report on an approach for extracting information on the 3D structure of an object by using extreme-ultraviolet (EUV) radiation. In this method, two EUV pulses hit an isolated 3D object simultaneously from different directions, generating independent coherent diffraction patterns, resulting in two distinct bidimensional projections after phase retrieval. These views are then used, in combination with a ray tracing algorithm, to retrieve information on the 3D structure. This EUV stereoscopic imaging approach, similar to the natural process of binocular vision, provides sub-µm spatial resolution and single-shot capability. Moreover, ultrafast time resolution and spectroscopy can be readily implemented, and a further extension to x-ray wavelengths can be envisioned as well.

Classical interpretation for the influence of XUV pulse width on the streaking time delay and the oscillation amplitude of the momentum shift

We numerically investigate both the streaking time delay and the oscillation amplitude of the momentum shift of the photoelectron and justify them physically by developing a classical model based on the weak field approximation. The streaking time delay is insensitive to the extreme ultraviolet (XUV) pulse duration, while the oscillation amplitude obviously reduces as the XUV duration increases. This XUV duration dependence is attributed to the ionization probability of electron at initial times other than the peak of the XUV pulse. We propagate the classical electron trajectories originating at different initial times in the coupled Coulomb-laser (IR) potential and average the momentum shift for each trajectory over the width of the XUV pulse. By extracting the streaking time delay and the oscillation amplitude from this averaged momentum shift, the classical model results and the time-dependent Schrödinger equation results are found to be in good agreement. Both the insensitivity of the streaking time delay and the sensitivity of the oscillation amplitude on the XUV pulse width are well explained by our classical model considering initial ionization time average. Analytical estimation for the oscillation amplitude is obtained from the model of initial ionization time average.

X-FAST: A versatile, high-throughput, and user-friendly XUV femtosecond absorption spectroscopy tabletop instrument.

We present the X-FAST (XUV Femtosecond Absorption Spectroscopy Tabletop) instrument at the University of Wisconsin-Madison. The instrument produces femtosecond extreme ultraviolet photon pulses via high-harmonic generation in the range of 40-72eV, as well as optical pump pulses for transient-absorption experiments. The system implements a gas-cooled sample cell that enables studying the dynamics of thermally sensitive thin-film samples. This paper provides potential users with specifications of the optical, vacuum, data acquisition, and sample cooling systems of the X-FAST instrument, along with performance metrics and data of an ultrafast laser-induced phase transition in a Ni2MnGa Heusler thin film.

Versatile and robust reconstruction of extreme-ultraviolet pulses down to the attosecond regime

A reliable and complete temporal characterization of ultrashort pulses is a crucial requisite for the correct interpretation of time-resolved experiments. This task is particularly challenging in the extreme-ultraviolet (XUV) spectral region, where usually different approaches are employed depending on the exact temporal structure of the pulses. Here we propose and validate against both simulated and experimental data a novel approach for the reconstruction of ultrashort XUV pulses produced by high-order harmonic generation in gases for three different conditions: isolated attosecond pulses, attosecond pulse trains, and few-femtosecond pulses obtained by spectral selection of single harmonics. The core of the method, named simplified trace reconstruction in the perturbative regime (STRIPE), is a novel mathematical description providing a simplified picture of the two-color photoionization process. This new approach is capable of accurately retrieving the temporal characteristics of the XUV pulses with notably reduced computational costs compared to other currently used reconstruction techniques. Direct comparison to standard approaches proves it to be superior in terms of flexibility, reliability, and robustness against noise and acquisition artifacts, making STRIPE a promising tool for pulse characterization.

Free electron laser stochastic spectroscopy revealing silicon bond softening dynamics

Time-resolved x-ray emission/absorption spectroscopy (Tr-XES/XAS) is an informative experimental tool sensitive to electronic dynamics in materials, widely exploited in diverse research fields. Typically, Tr-XES/XAS requires x-ray pulses with both a narrow bandwidth and subpicosecond pulse duration, a combination that in principle finds its optimum with Fourier transform-limited pulses. In this work, we explore an alternative experimental approach, capable of simultaneously retrieving information about unoccupied (XAS) and occupied (XES) states from the stochastic fluctuations of broadband extreme ultraviolet pulses of a free electron laser. We used this method, in combination with singular-value decomposition and Tikhonov regularization procedures, to determine the XAS/XES response from a crystalline silicon sample at the ${L}_{2,3}$ edge, with an energy resolution of a few tens of meV. Finally, we combined this spectroscopic method with a pump-probe approach to measure structural and electronic dynamics of a silicon membrane. Tr-XAS/XES data obtained after photoexcitation with an optical laser pulse at 390 nm allowed us to observe perturbations of the band structure, which are compatible with the formation of the predicted precursor state of a nonthermal solid-liquid phase transition associated with a bond softening phenomenon.

Free-electron laser temporal diagnostic beamline FL21 at FLASH.

A beamline for temporal diagnostics of extreme ultraviolet (XUV) femtosecond pulses at the free-electron laser in Hamburg (FLASH) at DESY was designed, built and put into operation. The intense ultra-short XUV pulses of FLASH fluctuate from pulse to pulse due to the underlying FEL operating principle and demand single-shot diagnostics. To cope with this, the new beamline is equipped with a terahertz field-driven streaking setup that enables the determination of single pulse duration and arrival time. The parameters of the beamline and the diagnostic setup as well as some first experimental results will be presented. In addition, concepts for parasitic operation are investigated.

Attosecond Real-Time Observation of Recolliding Electron Trajectories in Helium at Low Laser Intensities.

Laser-driven recollision physics is typically accessible only at field intensities high enough for tunnel ionization. Using an extreme ultraviolet pulse for ionization and a near-infrared (NIR) pulse for driving of the electron wave packet lifts this limitation. This allows us to study recollisions for a broad range of NIR intensities with transient absorption spectroscopy, making use of the reconstruction of the time-dependent dipole moment. Comparing recollision dynamics with linear vs circular NIR polarization, we find a parameter space, where the latter favors recollisions, providing evidence for the so far only theoretically predicted recolliding periodic orbits.

Spectrally tunable ultrashort monochromatized extreme ultraviolet pulses at 100 kHz

We present the experimental realization of spectrally tunable, ultrashort, quasi-monochromatic extreme ultraviolet (XUV) pulses generated at 100 kHz repetition rate in a user-oriented gas high harmonic generation beamline of the Extreme Light Infrastructure—Attosecond Light Pulse Source facility. Versatile spectral and temporal shaping of the XUV pulses is accomplished with a double-grating, time-delay compensated monochromator accommodating the two composing stages in a novel, asymmetrical geometry. This configuration supports the achievement of high monochromatic XUV flux (2.8 ± 0.9 × 1010 photons/s at 39.7 eV selected with 700 meV full width at half maximum bandwidth) combined with ultrashort pulse duration (4.0 ± 0.2 fs using 12.1 ± 0.6 fs driving pulses) and small spot size (sub-100 µm). Focusability, spectral bandwidth, and overall photon flux of the produced radiation were investigated, covering a wide range of instrumental configurations. Moreover, complete temporal (intensity and phase) characterization of the few-femtosecond monochromatic XUV pulses—a goal that is difficult to achieve by conventional reconstruction techniques—has been realized using a ptychographic algorithm on experimentally recorded XUV-infrared pump–probe traces. The presented results contribute to in situ, time-resolved experiments, accessing direct information on the electronic structure dynamics of novel target materials.