XUV Photon Energy Research Articles

Two-XUV-photon double ionization of neon

Two-XUV-photon double ionization of Ne, induced by an intense few-pulse attosecond train with a \ensuremath{\sim}4 fs envelope duration is investigated experimentally and theoretically. The experiment is performed at ELI-ALPS (Extreme Light Infrastructure Attosecond Light Pulse Source) utilizing the recently constructed 10 Hz gas phase high-order harmonic generation SYLOS GHHG-COMPACT beamline. A total pulse energy up to \ensuremath{\sim}1 \ensuremath{\mu}J generated in argon in conjunction with high-reflectivity optics in the XUV region allowed the observation of the doubly charged state of Ne induced by 40 eV central XUV-photon energies. The interaction of the intense attosecond pulse train with Ne is also theoretically studied via second-order time-dependent perturbation theory equations of motion. The results of this work, combined with the feasibility of conducting XUV-pump--XUV-probe experiments, constitute a powerful tool for many potential applications. Those include attosecond pulse metrology as well as time-resolved investigations of the dynamics underlying direct and sequential double ionization and their electron correlation effects.

Roles of the transition amplitude phases in photoelectron asymmetry of single strong attosecond pulse

The angular distributions of the photoelectrons in ionization of hydrogen atom by both circularly and linearly polarized intense extreme ultraviolet (XUV) attosecond pulse are investigated by numerically solving the time-dependent Schrödinger equation. We clearly identify nonperturbative features in studying the asymmetrical photoelectron angular distributions in the polarization plane for the XUV photon energy (16.3 eV) close to the ionization threshold, while such nonperturbative features are absent for higher photon energy (36 eV) in the same pulse intensity region. In addition to the carrier-envelope phase (CEP) dependence, the ejection asymmetry of the photoelectron is also sensitive to the relative phases of transition amplitudes in absorbing one photon and two photons. As a consequence, the CEPs corresponding to the maximal (or zero) asymmetry obviously vary as the pulse intensity increases in a moderately large region from 1 × 1015 W cm−2 to 30 × 1015 W cm−2. We attribute the intensity dependence of the transition amplitude phases to a consequence of the depletion of population as well as the Stark energy shift of the initial state. We show that the relative phases of transition amplitudes can be precisely decoded from the pulse intensity dependence of the ejection asymmetry and those phases are insensitive to the ellipticity of the laser pulse.

Analysis of RABITT time delays using the stationary multiphoton molecular R -matrix approach

We employ the recently developed multiphoton $R$-matrix method for molecular above-threshold photoionization to obtain second-order ionization amplitudes that govern the interference in RABITT experiments. This allows us to extract RABITT time delays that are in better agreement with nonperturbative time-dependent simulations of this process than the typically used combination of first-order (Wigner) delays and asymptotic corrections. We calculate molecular-frame as well as orientation-averaged RABITT delays for ${\mathrm{H}}_{2}, {\mathrm{N}}_{2}, {\mathrm{CO}}_{2}, {\mathrm{H}}_{2}\mathrm{O}$, and ${\mathrm{N}}_{2}\mathrm{O}$ and analyze the origin of various structures in the time delays including the effects of partial-wave interference, shape resonances, and orientation averaging. Time delays for B and C states of ${\mathrm{CO}}_{2}{}^{+}$ are strongly affected by absorption of the second (IR) photon in the ion. This effect corresponds to an additional contribution ${\ensuremath{\tau}}_{\text{coupl}}$ to the asymptotic approximation for the RABITT delays $\ensuremath{\tau}\ensuremath{\approx}{\ensuremath{\tau}}_{\text{mol}}+{\ensuremath{\tau}}_{cc}+{\ensuremath{\tau}}_{\text{coupl}}$. Applicability of the asymptotic theory depends on the target and IR photon energy but typically starts at approximately 30--35 eV of XUV photon energy.

Linear dichroism in few-photon ionization of laser-dressed helium

Ionization of laser-dressed atomic helium is investigated with focus on photoelectron angular distributions stemming from two-color multi-photon excited states. The experiment combines extreme ultraviolet (XUV) with infrared (IR) radiation, while the relative polarization and the temporal delay between the pulses can be varied. By means of an XUV photon energy scan over several electronvolts, we get access to excited states in the dressed atom exhibiting various binding energies, angular momenta, and magnetic quantum numbers. Furthermore, varying the relative polarization is employed as a handle to switch on and off the population of certain states that are only accessible by two-photon excitation. In this way, photoemission can be suppressed for specific XUV photon energies. Additionally, we investigate the dependence of the photoelectron angular distributions on the IR laser intensity. At our higher IR intensities, we start leaving the simple multi-photon ionization regime. The interpretation of the experimental results is supported by numerically solving the time-dependent Schrödinger equation in a single-active-electron approximation.Graphic abstract

Extreme ultraviolet photon effect on ionization and recombination of high-order harmonic generation

The extreme ultraviolet (XUV) pulse effect on the ionization and recombination of the high-order harmonic generation has been theoretically studied. It is shown that (i) with the introduction of a shorter duration XUV pulse to a fundamental infrared (IR) pulse, the XUV photon can only be absorbed during the electron ionization process. Thus, the harmonic signal can be enhanced due to the XUV resonance transition and ionization. (ii) With the introduction of a longer-duration XUV pulse to a fundamental IR pulse, the XUV photon can be absorbed not only in the electron ionization process, but also in the electron recombination process. As a result, not only the harmonic signal can be improved, but also the harmonic cutoff can be extended with an additional XUV photon energy region (. Moreover, as the XUV intensity increases, much more XUV photons can be absorbed in the electron recombination process, thus leading to the harmonic cutoff extension with the extra photon energy region of .

Photoelectron spectroscopy of laser-dressed atomic helium

Photoelectron emission from excited states of laser-dressed atomic helium is analyzed with respect to laser intensity-dependent excitation energy shifts and angular distributions. In the two-color XUV (exteme ultra\-violet) -- IR (infrared) measurement, the XUV photon energy is scanned between \SI{20.4}{\electronvolt} and the ionization threshold at \SI{24.6}{\electronvolt}, revealing electric dipole-forbidden transitions for a temporally overlapping IR pulse ($\sim\!\SI{e12}{\watt\per \centi\meter\squared}$). The interpretation of the experimental results is supported by numerically solving the time-dependent Schr\"odinger equation in a single-active-electron approximation.

Enhanced polarization transfer to the characteristic Lα x-ray lines near the nonlinear Cooper minimum of two-photon ionization

It has been shown that for nonlinear atomic ionization, transfer of the degree of circular polarization from incident to fluorescence light is maximum at the Cooper minimum [J. Hofbrucker, A. V. Volotka, and S. Fritzsche, Phys. Rev. A 100, 011401(R) (2019)]. However, it is still a challenge to produce and detect circularly polarized light at xuv and x-ray photon energies. We here show that transfer of linear polarization is strongly enhanced at the Cooper minimum in two-photon ionization and can be readily detected using current free-electron laser facilities by measurements of the degree of linear polarization of the characteristic $L{\ensuremath{\alpha}}_{1}$ and $L{\ensuremath{\alpha}}_{2}$ lines. Two-photon ionization of a $2{p}_{3/2}$ electron of a tungsten atom is proposed to demonstrate the presented phenomena and realization of such an experiment is discussed in detail.

Selection of the magnetic quantum number in resonant ionization of neon using an XUV–IR two-color laser field

A recent experiment (Villeneuve et al 2017 Science 356 1150) has shown that two-color photoionization of neon by the combination of an attosecond XUV pulse train and a moderately strong, linearly polarized IR pulse can preferentially produce photoelectrons with orbital angular quantum number l = 3 (f-wave) and magnetic quantum number m = 0. This result was rationalized by the occurrence of different Stark shifts of m = 0 and |m| = 1 sub-levels in the IR laser field. Here we perform 3D time-dependent Schrödinger equation calculations with a neon effective potential to identify the mechanism for the selective excitation and ionization of m = 0 sub-levels. Calculations of the ionization and excitation yields as a function of the IR intensity and the XUV and IR photon energy reveal that a coupling between two dominant ionization channels involving 3p and 3d intermediate excitations is responsible for the observed m-level selectivity. We compare calculated and measured photoelectron velocity map images and ionization yields over a range of IR intensities and XUV and IR photon energies, and confirm that the m = 0 or |m| = 1 channel, and thus a single set of the quantum numbers, (Jion, l, m), can be selected by an appropriate choice of these parameters.

Abnormal photoelectron angular distribution of Ar atoms in pulsed XUV and IR laser fields

SynopsisWe calculated the photoelectron angular distribution of Ar atoms in pulsed XUV and IR laser fields by solving the time-dependent Schrödinger equation and found that the angular distributions of sidebands are not always straight lines in the energy-angle plot as predicted by the strong field approximation. Further study shows that the abnormality is attributed to the photoelectron-nucleus Coulomb interaction. The abnormality depends on the IR intensity, IR pulse duration, XUV photon energy and the time-delay between the two pulses.

Dissociative photoionization of NO across a shape resonance in the XUV range using circularly polarized synchrotron radiation.

We report benchmark results for dissociative photoionization (DPI) spectroscopy and dynamics of the NO molecule in the region of the σ* shape resonance in the ionization leading to the NO+(c3Π) ionic state. The experimental study combines well characterized extreme ultraviolet (XUV) circularly polarized synchrotron radiation, delivered at the DESIRS beamline (SOLEIL), with ion-electron coincidence 3D momentum spectroscopy. The measured (N+, e) kinetic energy correlation diagrams reported at four discrete photon energies in the extended 23-33 eV energy range allow for resolving the different active DPI reactions and underline the importance of spectrally resolved studies using synchrotron radiation in the context of time-resolved studies where photoionization is induced by broadband XUV attosecond pulses. In the dominant DPI reaction which leads to the NO+(c3Π) ionic state, photoionization dynamics across the σ* shape resonance are probed by molecular frame photoelectron angular distributions where the parallel and perpendicular transitions are highlighted, as well as the circular dichroism CDAD(θe) in the molecular frame. The latter also constitute benchmark references for molecular polarimetry. The measured dynamical parameters are well described by multichannel Schwinger configuration interaction calculations. Similar results are obtained for the DPI spectroscopy of highly excited NO+ electronic states populated in the explored XUV photon energy range.

Nonlinear XUV-optical transient grating spectroscopy at the Si L2,3–edge

Time-resolved transient grating (TG) spectroscopy facilitates detailed studies of electron dynamics and transport phenomena by means of a periodic excitation of matter with coherent ultrashort light pulses. Several current and next generation free-electron laser (FEL) facilities provide fully coherent pulses with few femtosecond pulse durations and extreme ultraviolet (XUV) photon energies. Thus, they allow for transient grating experiments with periodicities as small as tens of nanometers and with element specific photon energies. Here, we demonstrate the element specificity of XUV TG (X-TG) experiments by tuning the photon energy across the Si L2,3-edge of Si3N4. We observe a shortening of the signal decay when increasing the XUV photon energy above the absorption edge. The analysis of the wavelength dependent signal shows that the faster decay is driven by the increase in the charge carrier density. From the decay constants the interband Auger coefficient at elevated temperatures and high electron densities has been determined.

Alignment of the aberration-free XUV Raman spectrometer at FLASH.

An extreme-ultraviolet (XUV) double-stage Raman spectrometer is permanently installed as an experimental end-station at the PG1 beamline of the soft X-ray/XUV free-electron laser in Hamburg, FLASH. The monochromator stages are designed according to the Czerny-Turner optical scheme, adapted for the XUV photon energy range, with optical elements installed at grazing-incidence angles. Such an optical scheme along with the usage of off-axis parabolic mirrors for light collimation and focusing allows for aberration-free spectral imaging on the optical axis. Combining the two monochromators in additive dispersion mode allows for reaching high resolution and superior stray light rejection, but puts high demands on the quality of the optical alignment. In order to align the instrument with the highest precision and to quantitatively characterize the instrument performance and thus the quality of the alignment, optical laser interferometry, Hartmann-Shack wavefront-sensing measurements as well as off-line soft X-ray measurements and extensive optical simulations were conducted. In this paper the concept of the alignment scheme and the procedure of the internal optical alignment are presented. Furthermore, results on the imaging quality and resolution of the first monochromator stage are shown.

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.

Ultrafast extreme ultraviolet photoemission without space charge.

Time- and Angle-resolved photoelectron spectroscopy from surfaces can be used to record the dynamics of electrons and holes in condensed matter on ultrafast time scales. However, ultrafast photoemission experiments using extreme-ultraviolet (XUV) light have previously been limited by either space-charge effects, low photon flux, or limited tuning range. In this article, we describe XUV photoelectron spectroscopy experiments with up to 5 nA of average sample current using a tunable cavity-enhanced high-harmonic source operating at 88 MHz repetition rate. The source delivers >1011 photons/s in isolated harmonics to the sample over a broad photon energy range from 18 to 37 eV with a spot size of 58 × 100 μm2. From photoelectron spectroscopy data, we place conservative upper limits on the XUV pulse duration and photon energy bandwidth of 93 fs and 65 meV, respectively. The high photocurrent, lack of strong space charge distortions of the photoelectron spectra, and excellent isolation of individual harmonic orders allow us to observe laser-induced modifications of the photoelectron spectra at the 10−4 level, enabling time-resolved XUV photoemission experiments in a qualitatively new regime.

XUV pulse effect on signal modulations of harmonic spectra from H $$_{2}^{+}$$ 2 + and T $$_{2}^{+}$$ 2 +

The effects of signal modulations on the molecular high-order harmonic generations in $$\hbox {H}_{2}^{+ }$$ and $$\hbox {T}_{2}^{+}$$ have been theoretically investigated. It is found that with the introduction of the XUV pulse, due to the absorption of the extra XUV photons in the recombination process, multiplateaus on the harmonic spectra, separated by the XUV photon energy can be found. Moreover, this multiplateau structure is insensitive to the wavelength of the XUV pulse. In shorter pulse duration, the intensities of the multiplateaus from $$\hbox {H}_{2}^{+}$$ are higher than those from $$\hbox {T}_{2}^{+}$$ ; while in longer pulse duration, the opposite results can be found. Finally, by changing the delay time of the XUV pulse, the signal modulations (including the amplitude and the frequency modulations) of the multiplateaus can be controlled.

Laser wakefield acceleration with high-power, few-cycle mid-IR lasers

The study of laser wakefield electron acceleration (LWFA) using mid-IR laser drivers is a promising path for future laser driven electron accelerators, when compared to traditional near-IR laser drivers operating at 0.8–1 μm central wavelength (λlaser), as the necessary vector potential (a0) for electron injection can be achieved with smaller laser powers due to the linear dependence on λlaser. In this work, we perform 2D PIC simulations on LWFA using few-cycle, high power (5–15 TW) laser systems with λlaser ranging from 0.88 to 10 μm. Such few-cycle systems are currently under development, aiming at Gas High Harmonics Generation applications, where the favorable λlaser2 scaling extends the range of the XUV photon energies. We keep a0 and ne∕ncr (ne being the plasma density and ncr the critical density for each λlaser) as common denominators in our simulations, allowing for comparisons between drivers with different λlaser, with respect to the accelerated electron beam energy, charge and conversion efficiency. While the electron energies are mainly dominated by the plasma dynamics, the laser to electron beam energy conversion efficiency shows significant enhancement with longer wavelength laser drivers.

Multiple cutoffs in high harmonic generation via multi-XUV-photon absorption

High harmonic generation (HHG) is one of the most fundamental processes in the interaction of strong laser fields with atoms and molecules. Because of wide applications of HHG, for example, imaging atomic or molecular orbitals, visualizing chemical reactions, synthesizing a single attosecond pulse, the HHG attracts huge attentions in both theories and experiments. The HHG can be explained by the famous three-step model:first, the laser field bends the Coulomb potential and the electron tunnels out; second, the electron is accelerated in the laser field and gains kinetic energy; Third, the energetic electron recombines with the parent ion and release its energy as high energetic photons. The HHG can be tailored by controlling the each step. In this paper, we conceive a strategy to control the third step. We simulate the HHG when He+ is exposed to the combined few-cycle Ti-Sapphire (800 nm) IR femtosecond laser pulse and XUV laser pulse by numerically solving the time dependent Schrdinger equation. The simulation shows that after the electron tunnels out and gains energies from the infrared laser field, extra XUV photons may be absorbed during the electron and parent ion recombination, contributing multiple cutoffs separated by XUV photon energies in the high harmonic spectrum. This scenario is confirmed by time-delay-dependent HHG in the time-frequency representation, and by the power scaling of the cutoffs' intensities as a function of the XUV intensity.

Dynamics of N2 Dissociation upon Inner-Valence Ionization by Wavelength-Selected XUV Pulses.

Ionization of nitrogen by extreme ultraviolet (XUV) light from the Sun has recently been recognized as an important driver of chemical reactions in the atmosphere of Titan. XUV photons with energies of 24 eV and above convert inert nitrogen molecules into reactive neutral and ionic fragments that initiate chemical reactions. Understanding the XUV-induced fragmentation poses significant challenges to modern theory owing to its ultrafast time scales, complex electronic rearrangements, and strong dependence on the XUV photon energy. Here, we apply femtosecond time-resolved photoelectron and photoion spectroscopy to study dissociative ionization of nitrogen, the most abundant molecule in Titan's atmosphere, at selected XUV photon energies using a table-top XUV time-compensating monochromator. We probe the resulting dynamics using a time-delayed infrared (IR) ionization pulse. Coupled with ab initio calculations, the results allow us to assign the major dissociation channels resulting from production of an inner-valence hole, with important implications for models of Titan's XUV-driven atmospheric chemistry.

Atomic delay in helium, neon, argon and krypton**Intended contribution to the ‘Special issue on ultrafast electron and molecular dynamics’ available at http://iopscience.iop.org/0953-4075/47/12.

Photoionization by an eXtreme UltraViolet (XUV) attosecond pulse train (APT) in the presence of an infrared pulse (RABBITT method) conveys information about the atomic photoionization delay. By taking the difference of the spectral delays between pairs of rare gases (Ar,He), (Kr,He) and (Ne,He) it is possible to eliminate in each case the larger group delay (‘attochirp’) associated with the APT itself and obtain the Ar, Kr and Ne Wigner delays referenced to model calculations of the He delay. In this work we measure how the delays vary as a function of XUV photon energy but we cannot determine the absolute delay difference between atoms due to lack of precise knowledge of the initial conditions. The extracted delays are compared with several theoretical predictions and the results are consistent within 30 as over the energy range from 10 to 50 eV. An ‘effective’ Wigner delay over all emission angles is found to be more consistent with our angle-integrated measurement near the Cooper minimum in Ar. We observe a few irregular features in the delay that may be signatures of resonances.

Interference structures in photoelectron spectra of atoms ionized by XUV pulses in the presence of a strong IR field

The dynamics of photoelectrons ionized by XUV pulses in the presence of a strong infrared (IR) field is theoretically investigated by solving the time-dependent Schr\odinger equation (TDSE). We study the ionization dynamics of He by an XUV pulse in the presence of a relatively strong IR laser field, which is different from the conventional attosecond streaking experiments where a rather weak IR field is applied. Comparing with the photoelectron spectra produced by the IR field only, we find the spectra ionized by the combined fields construct interesting interference structures for different XUV photon energies and pulse intensities. These features can be analyzed and explained by a quantum-trajectory theory based on the strong-field approximation (SFA). The SFA theory shows excellent agreement with the TDSE results, revealing that these structures originate from interferences among photoelectrons ionized by XUV pluses (streaked by the strong IR field) at different moments, and in some energy regions, together with the photoelectrons ionized by the intense IR pulse itself.