Extreme Ultraviolet Laser Pulses Research Articles

The Role of Momentum Partitioning in Covariance Ion Imaging Analysis.

We present results from a covariance ion imaging study, which employs extensive filtering, on the relationship between fragment momenta to gain deeper insight into photofragmentation dynamics. A new data analysis approach is introduced that considers the momentum partitioning between the fragments of the breakup of a molecular polycation to disentangle concurrent fragmentation channels, which yield the same ion species. We exploit this approach to examine the momentum exchange relationship between the products, which provides direct insight into the dynamics of molecular fragmentation. We apply these techniques to extensively characterize the dissociation of 1-iodopropane and 2-iodopropane dications prepared by site-selective ionization of the iodine atom using extreme ultraviolet intense femtosecond laser pulses with a photon energy of 95 eV. Our assignments are supported by classical simulations, using parameters largely obtained directly from the experimental data.

A high-efficiency programmable modulator for extreme ultraviolet light with nanometre feature size based on an electronic phase transition

AbstractThe absence of efficient light modulators for extreme ultraviolet (EUV) and X-ray photons considerably limits their real-life application, particularly when even slight complexity of the beam patterns is required. Here we report on a novel approach to reversible imprinting of a holographic mask in an electronic Wigner crystal material with a sub-90-nm feature size. The structure is imprinted on a sub-picosecond timescale using EUV laser pulses, and acts as a high-efficiency diffraction grating that deflects EUV or soft X-ray light. The imprinted nanostructure is stable after the removal of the exciting beams at low temperatures, but can be easily erased by a single heating beam. Modelling shows that the efficiency of the device can exceed 1%, approaching state-of-the-art etched gratings, but with the benefit of being programmable and tunable over a large range of wavelengths. The observed effect is based on the rapid change of lattice constant upon transition between metastable electronically ordered phases in a layered transition metal dichalcogenide. The proposed approach is potentially useful for creating tunable light modulators in the EUV and soft X-ray spectral ranges.

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.

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.

Photon Acceleration from Optical to XUV.

The propagating density gradients of a plasma wakefield may frequency upshift a trailing witness laser pulse, a process known as "photon acceleration." In uniform plasma, the witness laser will eventually dephase because of group delay. We find phase-matching conditions for the pulse using a tailored density profile. An analytic solution for a 1D nonlinear plasma wake with an electron beam driver indicates that, even though the plasma density decreases, the frequency shift reaches no asymptotic limit, i.e., is unlimited provided the wake can be sustained. In fully self-consistent 1D particle-in-cell (PIC) simulations, more than 40 times frequency shifts were demonstrated. In quasi-3D PIC simulations, frequency shifts up to 10 times were observed, limited only by simulation resolution and nonoptimized driver evolution. The pulse energy increases in this process, by a factor of 5, and the pulse is guided and temporally compressed by group velocity dispersion, resulting in the resulting extreme ultraviolet laser pulse having near-relativistic (a_{0}∼0.4) intensity.

Molecular photodissociation dynamics revealed by Coulomb explosion imaging.

Coulomb explosion imaging (CEI) methods are finding ever-growing use as a means of exploring and distinguishing the static stereo-configurations of small quantum systems (molecules, clusters, etc). CEI experiments initiated by ultrafast (femtosecond-duration) laser pulses also allow opportunities to track the time-evolution of molecular structures, and thereby advance understanding of molecular fragmentation processes. This Perspective illustrates two emerging families of dynamical studies. 'One-colour' studies (employing strong field ionisation driven by intense near infrared or single X-ray or extreme ultraviolet laser pulses) afford routes to preparing multiply charged molecular cations and exploring how their fragmentation progresses from valence-dominated to Coulomb-dominated dynamics with increasing charge and how this evolution varies with molecular size and composition. 'Two-colour' studies use one ultrashort laser pulse to create electronically excited neutral molecules (or monocations), whose structural evolution is then probed as a function of pump-probe delay using an ultrafast ionisation pulse along with time and position-sensitive detection methods. This latter type of experiment has the potential to return new insights into not just molecular fragmentation processes but also charge transfer processes between moieties separating with much better defined stereochemical control than in contemporary ion-atom and ion-molecule charge transfer studies.

Submicron structures created on Ni thin film by submicron focusing of femtosecond EUV light pulses

Using a newly developed submicron focusing system equipped with a large-aperture Wolter mirror with a precisely figured surface, we irradiate a Ni thin film coated on a silicon substrate with femtosecond extreme ultraviolet (EUV) laser pulses, generated as high-order harmonics of near-infrared femtosecond laser pulses. At the fluence of up to 100 mJ cm−2 at the sample surface, we show that the surface morphology can be modified with a submicron spatial resolution and that a protruding structure is formed when the fluence is 60–70 mJ cm−2, exhibiting a characteristic feature of the femtosecond EUV light processing of a thin metal surface.

Ion-photoelectron entanglement in photoionization with chirped laser pulses

The investigation of coherent dynamics induced by photoionization of atoms or molecules by extreme ultra-violet (XUV) attosecond laser pulses requires careful consideration of the degree of ion + photoelectron entanglement that results from the photoionization process. Here, we consider coherent H2 + vibrational dynamics induced by photoionization of neutral H2 by a chirped attosecond laser pulse. We show that chirping the attosecond laser pulse leads to ion + photoelectron entanglement and the transition from a pure to a mixed state. This transition is characterized by evaluating the purity, which is close to unity for a transform-limited attosecond laser pulse and which decreases to a value that is determined by the number of vibrational states populated in the photoionization process for increasing values of the chirp parameter. In the calculations, the vibrational dynamics is probed by calculating time-delayed dissociation of the H2 + cation by a short ultra-violet (UV) laser pulse. Independent of the magnitude of the chirp, the coherent vibrational dynamics can be recovered by recording the XUV-UV delay-dependent kinetic energy release in coincidence with the kinetic energy of the accompanying photoelectron.

Laser-Induced Electron Fresnel Diffraction in Tunneling and Over-Barrier Ionization

Photoelectron momentum distribution in strong-field ionization has a variety of structures that reveal the complicated dynamics of this process. Recently, we identified a low-energy interference structure in the case of a super-intense extreme ultraviolet (XUV) laser pulse and attributed it to the laser-induced electron Fresnel diffraction. This structure is determined by the laser-induced electron displacement [Geng et al. Phys. Rev. A 104 (2021) L021102]. In the present work, we find that the Fresnel diffraction picture also appears in the tunneling and over-barrier regime of ionization by short pulses. However, the electron displacement is now induced by the electric field component of the laser pulse rather than the magnetic field component in the case of the super-intense XUV pulse. After corresponding modifications to our quantum and semiclassical models, we find that the same physical mechanism of the Fresnel diffraction governs the low-energy interference structures along the laser polarization. The results predicted by the two models agree well with the accurate results from the numerical solution to the time-dependent Schrödinger equation.

Experimental Control of Quantum-Mechanical Entanglement in an Attosecond Pump-Probe Experiment.

Entanglement is one of the most intriguing aspects of quantum mechanics and lies at the heart of the ongoing second quantum revolution, where it is a resource that is used in quantum key distribution, quantum computing, and quantum teleportation. We report experiments demonstrating the crucial role that entanglement plays in pump-probe experiments involving ionization, which are a hallmark of the novel research field of attosecond science. We demonstrate that the degree of entanglement in a bipartite ion + photoelectron system, and, as a consequence, the degree of vibrational coherence in the ion, can be controlled by tailoring the spectral properties of the attosecond extreme ultraviolet laser pulses that are used to create them.

On the mechanisms of the influence of preliminary ionization on the plasma dynamics of nanosecond capillary discharges and the properties of discharge-based EUV lasers

In this paper, we present the results of numerical investigations into the influence of preionization on the properties of extreme ultraviolet (EUV) lasers based on nanosecond capillary discharges. Prior to application of the main current pulse, gas inside the capillary is usually preionized by a separate current pulse with longer duration and lower amplitude, which creates plasma with minimal density on the capillary axis and maximal at the capillary wall. Magnetohydrodynamic simulations were performed for a range of prepulse parameters that defined different degrees of inhomogeneity of this initial profile. It was found that the plasma density distribution at the start of the main current pulse affects the cylindrical shock wave that takes place during the compression stage of a capillary discharge: A lower degree of radial inhomogeneity results in a steeper front of the shock wave. It is further shown that a steeper wave front results in a more concave electron density profile moments before the shock wave collapses on the capillary axis, when the EUV laser pulse presumably takes place, which may lead to a decrease in the rate of refraction losses. The proposed interpretation of the obtained numerical results correlates well with the available experimental data on the dependence of EUV laser pulse intensity and duration on the preliminary pulse amplitude.

Laser-induced electron Fresnel diffraction by XUV pulses at extreme intensity

Ionization of atoms and molecules in laser fields can lead to various interesting interference structures in the photoelectron spectrum. For the case of a superintense extreme ultraviolet laser pulse, we identify a novel petal-like interference structure in the electron momentum distribution along the direction of the laser field propagation. We show that this structure is quite general and can be attributed to the Fresnel diffraction of the electronic wave packet by the nucleus. Our results are demonstrated by numerically solving the time-dependent Schr\"odinger equation of the atomic hydrogen beyond the dipole approximation. By building an analytical model, we find that the electron displacement determines the aforementioned interference pattern. In addition, we establish the physical picture of laser-induced electron Fresnel diffraction which is reinforced by both quantum and semiclassical models.

Solving the time-dependent Schrödinger equation by combining smooth exterior complex scaling and Arnoldi propagator

We develop a highly efficient scheme for numerically solving the three-dimensional time-dependent Schrödinger equation of the single-active-electron atom in the field of laser pulses by combining smooth exterior complex scaling (SECS) absorbing method and Arnoldi propagation method. Such combination has not been reported in the literature. The proposed scheme is particularly useful in the applications involving long-time wave propagation. The SECS is a wonderful absorber, but its application results in a non-Hermitian Hamiltonian, invalidating propagators utilizing the Hermitian symmetry of the Hamiltonian. We demonstrate that the routine Arnoldi propagator can be modified to treat the non-Hermitian Hamiltonian. The efficiency of the proposed scheme is checked by tracking the time-dependent electron wave packet in the case of both weak extreme ultraviolet (XUV) and strong infrared (IR) laser pulses. Both perfect absorption and stable propagation are observed.

All-optical single-shot complete electric field measurement of extreme ultraviolet free electron laser pulses

Recent advances in ultrafast extreme ultraviolet (EUV) and x-ray light sources provide direct access to fundamental time and length scales for biology, chemistry, and materials physics. However, such light pulses are challenging to measure due to the need for femtosecond time resolution at difficult-to-detect wavelengths. Also, single-shot measurements are needed because severe pulse-to-pulse fluctuations are common. Here we demonstrate single-shot, complete field measurements by applying a novel version of frequency resolved optical gating. An EUV free electron laser beam creates a transient grating containing the pulse’s electric field information, which is read out with a 400 nm probe pulse. By varying the time delay between two copies of the EUV pump, rather than between the pump and the probe, we separate the needed coherent wave mixing from the slow incoherent response. Because this approach uses photoionization, it should be applicable from the vacuum ultraviolet to hard x rays.

Control of Attosecond Entanglement and Coherence.

Calculations are presented of vibrational wave packet dynamics in H_{2}^{+} ions formed by ionization of neutral H_{2} by a pair of attosecond extreme ultraviolet laser pulses, using time-delayed dissociation of the cation by an ultraviolet probe pulse. The strength of experimentally observable two-level quantum beats as a function of the attosecond two-pulse delay can be related to ion+photoelectron entanglement resulting from the ionization process. This conclusion is supported by an evaluation of the purity of the reduced ion and photoelectron density matrices.

Photoionization of aligned excited states in neon by attosecond laser pulses

We numerically describe the ionization process induced by linearly and circularly polarized extreme ultraviolet (XUV) attosecond laser pulses on an aligned atomic target, specifically the excited state Ne*(1s 22s 22p 5[]3s[]). We compute the excited atomic state by applying the time-dependent restricted-active-space self-consistent field method to fully account for the electronic correlation. We find that correlation-assisted ionization channels can dominate channels accessible without correlation. We also observe that the rotation of the photoelectron momentum distribution by circularly polarized laser pulses compared to the case of linear polarization can be explained in terms of differences in accessible ionization channels. This study shows that it is essential to include electron correlation effects to obtain an accurate description of the photoelectron emission dynamics from aligned excited states.

High resolution time- and angle-resolved photoemission spectroscopy with 11 eV laser pulses.

Performing time- and angle-resolved photoemission (tr-ARPES) spectroscopy at high momenta necessitates extreme ultraviolet laser pulses, which are typically produced via high harmonic generation (HHG). Despite recent advances, HHG-based setups still require large pulse energies (from hundreds of μJ to mJ) and their energy resolution is limited to tens of meV. Here, we present a novel 11 eV tr-ARPES setup that generates a flux of 5 × 1010 photons/s and achieves an unprecedented energy resolution of 16 meV. It can be operated at high repetition rates (up to 250 kHz) while using input pulse energies down to 3 µJ. We demonstrate these unique capabilities by simultaneously capturing the energy and momentum resolved dynamics in two well-separated momentum space regions of a charge density wave material ErTe3. This novel setup offers the opportunity to study the non-equilibrium band structure of solids with exceptional energy and time resolutions at high repetition rates.

Ionization of helium by an ultrashort extreme-ultraviolet laser pulse

We theoretically study photoelectron angular distributions and related anisotropy parameters for the competition of one- and two-photon ionization of He in an ultrashort extreme-ultraviolet laser pulse, using numerical results from the time-dependent Schrödinger equation. We explore the transition between the two processes for variation of the pulse duration, peak intensity, and central frequency or photoelectron energy. In the results obtained for fixed pulse parameters the transition and interference between the processes can be observed in the even (β2, β4) and odd (β1, β3) parameters, respectively, while the onset of the impact of three-photon ionization is observed via β5 at high peak intensities. Finally, we show that the transition can be observed via the even anisotropy parameters in pulses without carrier-to-envelope stabilization as well as in free-electron laser pulses with fluctuating pulse shape.

Two-Electron Interference in Strong-Field Ionization of He by a Short Intense Extreme Ultraviolet Laser Pulse.

Double ionization of helium by a single intense (above 10^{18} W/cm^{2}) linearly polarized extreme ultraviolet laser pulse is studied by numerically solving the full-dimensional time-dependent Schrödinger equation. For the laser intensities well beyond the perturbative limit, novel gridlike interference fringes are found in the correlated energy spectrum of the two photoelectrons. The interference can be traced to the multitude of two-electron wave packets emitted at different ionization times. A semianalytical model for the dressed two-photon double ionization is shown to qualitatively account for the interference patterns in the joint energy spectrum. Similar signatures of interferences between transient induced time-delayed ionization bursts are expected for other atomic and molecular multielectron systems.

Ultrafast time-resolved photoelectron and ion fragment momentum imaging of vacuum ultraviolet-excited molecules

SynopsisNew experimental results are presented on the dissociation dynamics of small neutral molecules in time-resolved photoexcitation-photoionization experiments by ultrashort vacuum- and extreme-ultraviolet laser pulses and charged particle momentum imaging.