Peer-Review Publications

The resonance 3C ([(2p(5))(1/2)3d(3/2)](J=1)->[2p(6)](J=0)) to intercombination 3D ([(2p(5))(3/2) 3d(5/2)](J=1)->[2p(6)](J=0)) line intensity ratio of neonlike ions has been studied. The measured line intensity ratio for neonlike Xe44+ ions shows an apparent change, which is reproduced by the calculations using the relativistic configuration interaction plus many-body perturbation theory. It is clearly elucidated that the change in the 3C/3D line intensity ratio is caused by strong configuration mixing between the upper levels of the 3D and 3F ([(2p(5))(1/2)3s](J=1)->[2p(6)](J=0)) lines. The present measurement allows us to discuss the 3C/3D line intensity ratio for the highest-Z ions hitherto, which suggests that the experiment-theory discrepancy in the 3C/3D line intensity ratio of neonlike ions diminishes with increasing atomic number Z and further trends to vanish at higher-Z ions. Furthermore, the present study provides benefits to better understand configuration mixing effect in the radiative opacity of hot plasmas. (C) 2022 Optica Publishing Group under the terms of the Optica Open Access Publishing Agreement

Coster-Kronig and super Coster-Kronig transitions from the Xe 4s core-hole state are investigated by coincidence detection of all the emitted electrons and product ions. The branching ratios of the transitions are determined by analyzing the coincidence data and comparing them to calculations. Subsequent decay pathways following these first-step Auger decays are also clarified.

We have conceived and built the HILITE (High-Intensity Laser-Ion Trap Experiment) Penning-trap setup for the production, confinement and preparation of pure ensembles of highly charged ions in a defined quantum state as a target for various high-intensity lasers. This enables a broad suite of laser-ion interaction studies at high photon energies and/or intensities, such as non-linear photo-ionisation studies. The setup has now been used to perform experiments at one such laser facility, namely the FLASH Free-Electron Laser at DESY in Hamburg, Germany. We describe the experimental possibilities of the apparatus, the results of the first measurements and future experiments at other laser facilities.

In the past, the ionization of atoms and molecules by strong, mid-infrared (IR) laser fields has attracted recurrent interest. Measurements with different IR pulses have demonstrated the crucial role of the magnetic field on the electron dynamics, classically known as the Lorentz force F-L = q (epsilon + v x B), that acts upon all particles with charge q in motion. These measurements also require the advancement of theory beyond the presently applied methods. In particular, the strong-field approximation (SFA) is typically based on the dipole approximation alone and neglects both the magnetic field and the spatial dependence of the driving electric field. Here we show and discuss that several, if not most, observations from strong-field ionization experiments with mid-IR fields can be quantitatively explained within the framework of SFA, if the Lorentz force is taken into account by nondipole Volkov states in the formalism. The details of such a treatment are analyzed for the (peak) shifts of the polar-angle distribution of above-threshold ionization photoelectrons along the laser propagation, the steering of electron momenta by two not quite collinear laser beams, or the enhanced momentum transfer to photoelectrons in standing-light fields. Moreover, the same formalism promises to explain the generation of high harmonics and other strong-field rescattering phenomena when driven by mid-IR laser fields. All these results show how strong-field processes can be understood on equal footings within the SFA, if one goes beyond the commonly applied dipole approximation.

Experimental cross sections for m-fold photodetachment (m = 2-5) of oxygen anions via K-shell excitation and ionization were measured in the photon-energy range of 525-1500 eV using the photon-ion merged-beams technique at a synchrotron light source. The measured cross sections exhibit clear signatures of direct double detachment, including double K-hole creation. The shapes of the double-detachment cross sections as a function of photon energy are in accord with Pattard s [J. Phys. B 35, L207 (2002)] empirical scaling law. We have also followed the complex de-excitation cascades that evolve subsequently to the initial double-detachment events by systematic large-scale cascade calculations. The resulting theoretical product charge-state distributions are in good agreement with the experimental findings.

We report on the generation of GW-class peak power, 35-fs pulses at 2-mu m wavelength with an average power of 51 W at 300-kHz repetition rate. A compact, krypton-filled Herriott-type cavity employing metallic mirrors is used for spectral broadening. This multi-pass compression stage enables the efficient post compression of the pulses emitted by an ultrafast coherently combined thulium-doped fiber laser system. The presented results demonstrate an excellent preservation of the input beam quality in combination with a power transmission as high as 80%. These results show that multi-pass cell based post-compression is an attractive alternative to nonlinear spectral broadening in fibers, which is commonly employed for thulium-doped and other mid-infrared ultra-fast laser systems. Particularly, the average power scalability and the potential to achieve few-cycle pulse durations make this scheme highly attractive. (C) 2022 Optica Publishing Group

The total ionization rate of biharmonic (omega + 3 omega) ionization is studied within the independent particle approximation and the third-order perturbation theory. Particular attention is paid to how the polarization of the biharmonic light field affects the total rate. The ratios of the biharmonic ionization rates for linearly and circularly polarized beams as well as for corotating and counter-rotating elliptically polarized beams are analyzed, and how they depend on the beam parameters, such as photon frequency or phase between omega and 3 omega light beams. We show that the interference of the biharmonic ionization amplitudes determines the dominance of a particular beam polarization over another and that it can be controlled by an appropriate choice of beam parameters. Furthermore, we demonstrate our findings for the ionization of neon L shell electrons.

An ab initio QED approach to treat a valence-hole excitation in closed-shell systems is developed in the framework of the two-time Greens-function method. The derivation considers a redefinition of the vacuum state and its excitation as a valence-hole pair. The proper two-time Greens function, whose spectral representation confirms the poles at valence-hole excitation energies, is proposed. An contour integral formula which connects the energy corrections and the Greens function is also presented. First-order corrections to the valence-hole excitation energy involving self-energy, vacuum polarization, and one-photon-exchange terms are explicitly derived in the redefined vacuum picture. Reduction to the usual vacuum electron propagators is shown, which agrees in the Breit approximation with the many-body perturbation theory expressions for the valence-hole excitation energy.

Post-compression of ultra-short laser pulses via self-phase modulation is routinely employed for the generation of laser pulses with optical bandwidths reaching far beyond the laser gain limitations. Although high compression factors can be routinely achieved, the compressed pulses typically suffer from temporal quality degradation. We numerically and experimentally analyze the deterioration of different measures of temporal quality with increasing compression factor and show how appropriate dispersion management and cascading of the post-compression process can be employed to limit the impact of this effect. The demonstrated saturation of pulse quality degradation at large compression factors puts novel femtosecond laser architectures based on post-compressed picosecond or even nanosecond laser systems in sight.

In Fourier ptychography, multiple lowresolution images are captured and subsequently combined computationally into a high-resolution, large-field of view micrograph. A theoretical image-formation model based on the assumption of plane-wave illumination from various directions is commonly used, to stitch together the captured information into a high synthetic aperture. The underlying far-field (Fraunhofer) diffraction assumption connects the source, sample, and pupil planes by Fourier transforms. While computationally simple, this assumption neglects phase-curvature due to non-planar illumination from point sources as well as phasecurvature from finite-conjugate microscopes (e.g., using a single-lens for image-formation). We describe a simple, efficient, and accurate extension of Fourier ptychography by embedding the effect of phase-curvature into the underlying forward model. With the improved forward model proposed here, quantitative phase reconstruction is possible even for wide fields-of-views and without the need of image segmentation. Lastly, the proposed method is computationally efficient, requiring only two multiplications: prior and following the reconstruction.

Electron-impact excitation from the ground state to the excited energy level 2p(3/2) of hydrogenlike ions and subsequent Lyman-alpha(1) (2p(3/2) -> 1s(1/2)) radiative decay are investigated using the relativistic distorted-wave method. Special attention is paid to the linear polarization and angular distribution of the Lyman-alpha(1) line and also to the effects of the Breit interaction. To this aim, detailed calculations are performed for hydrogenlike Ti21+, Mo41+, Ba55+, and Au78+ ions. It is found that the presently obtained (partial cross sections and) linear polarization agree excellently with other theoretical and experimental results available for low-Z Ti21+ ions within the experimental uncertainties. Moreover, the Lyman-alpha(1) line is found to be less linearly polarized and less anisotropic due to the contribution of the Breit interaction. Such effects of the Breit interaction behave more prominently for higher-Z ions and higher impact electron energies, respectively. For instance, the Breit interaction qualitatively changes the polarization behavior and angular emission pattern of the Lyman-alpha(1) line from high-Z Au78+ ions at the impact energy of about 4.2 times the corresponding excitation threshold.

Here, we use x-rays to create and probe quantum coherence in the photoionized amino acid glycine. The outgoing photoelectron leaves behind the cation in a coherent superposition of quantum mechanical eigenstates. Delayed x-ray pulses track the induced coherence through resonant x-ray absorption that induces Auger decay and by photoelectron emission from sequential double photoionization. Sinusoidal temporal modulation of the detected signal at early times (0 to 25 fs) is observed in both measurements. Advanced ab initio many-electron simulations allow us to explain the first 25 fs of the detected coherent quantum evolution in terms of the electronic coherence. In the kinematically complete x-ray absorption measurement, we monitor its dynamics for a period of 175 fs and observe an evolving modulation that may implicate the coupling of electronic to vibronic coherence at longer time scales. Our experiment provides a direct support for the existence of long-lived electronic coherence in photoionized biomolecules.

Scale deposition is the accumulation of various materials in the walls of transmission lines and unwanted parts in the oil and gas production system. It is a leading moot point in all transmission lines, tanks, and petroleum equipment. Scale deposition leads to drastic detrimental problems, reduced permeability, pressure and production losses, and direct financial losses due to the failure of some equipment. The accumulation of oil and gas leads to clogged pores and obstruction of fluid flow. Considering the passage of a two-phase flow, our study determines the thickness of the scale, and the flow regime is detected with the help of two Multilayer Perceptron (MLP) networks. First, the diagnostic system consisting of a dual-energy source, a steel pipe, and a NaI detector was implemented, using the Monte Carlo N Particle Code (MCNP). Subsequently, the received signals were processed, and properties were extracted using the wavelet transform technique. These features were considered as inputs of an Artificial Neural Network (ANN) model used to determine the type of flow regimes and predict the scale thickness. By accurately classifying the flow regimes and determining the scale inside the pipe, our proposed method provides a platform that could enhance many areas of the oil industry.

Quantum electrodynamics (QED) is one of the most fundamental theories of physics and has been shown to be in excellent agreement with experimental results(1-5). In particular, measurements of the electron\textquotesingle s magnetic moment (orgfactor) of highly charged ions in Penning traps provide a stringent probe for QED, which allows testing of the standard model in the strongest electromagnetic fields(6). When studying the differences between isotopes, many common QED contributions cancel owing to the identical electron configuration, making it possible to resolve the intricate effects stemming from the nuclear differences. Experimentally, however, this quickly becomes limited, particularly by the precision of the ion masses or the magnetic field stability(7). Here we report on a measurement technique that overcomes these limitations by co-trapping two highly charged ions and measuring the difference in their g factors directly. We apply a dual Ramsey-type measurement scheme with the ions locked on a common magnetron orbit(8), separated by only a few hundred micrometres, to coherently extract the spin precession frequency difference. We have measured the isotopic shift of the bound-electrongfactor of the isotopes Ne-20(9+) and Ne-22(9+) to 0.56-parts-per-trillion (5.6 x 10(-13)) precision relative to their g factors, an improvement of about two orders of magnitude compared with state-of-the-art techniques(7). This resolves the QED contribution to the nuclear recoil, accurately validates the corresponding theory and offers an alternative approach to set constraints on new physics.

Experimental and theoretical results are presented for double, triple, and quadruple photoionization of Si+ and Si2+ ions and for double photoionization of Si3+ ions by a single photon. The experiments employed the photon-ion merged-beams technique at a synchrotron light source. The experimental photon-energy range 1835-1900 eV comprises resonances associated with the excitation of a 1s electron to higher subshells and subsequent autoionization. Energies, widths, and strengths of these resonances are extracted from high-resolution photoionization measurements, and the core-hole lifetime of K-shell ionized neutral silicon is inferred. In addition, theoretical cross sections for photoabsorption and multiple photoionization were obtained from large-scale multiconfiguration Dirac-Hartree-Fock calculations. The present calculations agree with the experiment much better than previously published theoretical results. The importance of an accurate energy calibration of laboratory data is pointed out. The present benchmark results are particularly useful for discriminating between silicon absorption in the gaseous and in the solid component (dust grains) of the interstellar medium.

Ions with multiple inner-shell vacancies frequently arise due to their interaction with different targets, such as (intense) light pulses, atoms, clusters or bulk material. They are formed, in addition, if highly charged ions approach surfaces and capture electrons at rather large distances. To explore the interaction of such hollow ions and their subsequent relaxation, photon spectra in different frequency regions have been measured and compared to calculations. To support these and related measurements, we here show within the framework of the Jena Atomic Calculator (JAC) how (additional) electrons in outer shells modify photon emission and lead to characteristic shifts in the observed spectra. Further, for highly charged Ar ions in KLm (m = 1 ... 8) configurations, we analyze the mean relaxation time for their stabilization into the different ground configurations. These examples demonstrate how a powerful and flexible toolbox such as JAC will be useful (and necessary) in order to model the photon and electron emission of ions as they occur not only near surfaces but also in astro-, atomic and plasma physics.

The advent of petawatt-class laser systems allows generating electromagnetic fields of unprecedented strength in a controlled environment, driving increasingly more efforts to probe yet unobserved processes through their interaction with the quantum vacuum. Still, the lowest intensity scale governing these effects lies orders of magnitude beyond foreseen capabilities, so that such endeavor is expected to remain extremely challenging. In recent years, however, plasma mirrors have emerged as a promising bridge across this gap, by enabling the conversion of intense infrared laser pulses into coherently focused Doppler harmonic beams lying in the X-UV range. In this work, we present predictions on the quantum vacuum signatures produced when such beams are focused to intensities between 1024 and 1028 W cm−2, specifically photon–photon scattering and electron–positron pair creation. These signatures are computed via the stimulated vacuum formalism, combined with a model of perfectly focused beam built from PIC-generated harmonics spectra, and implemented on state-of-the-art massively parallel numerical tools. In view of identifying experimentally favorable configurations, we also consider the coupling of the focused harmonic beam with an auxiliary optical beam, and provide comparison with other established schemes. Our results show that a single coherently focused harmonic beam can produce as much scattered photons as two infrared pulses in head-on collision, and confirm that the coupling of the harmonic beam to an auxiliary beam gives rise to significant levels of inelastic scattering, and hence holds the potential to strongly improve the attainable signal to noise ratios in experiments.

The spontaneous crystal surface reconstruction of M-plane alpha-Al2O3 is employed for nanopatterning and nanofabrication in various fields of research including, among others, magnetism, superconductivity, and optoelectronics. In this reconstruction process the crystalline surface transforms from a planar morphology to one with a nanoscale ripple patterning. However, the high sample temperature required to induce surface reconstruction made in situ studies of the process seem unfeasible. The kinetics of ripple pattern formation therefore remained uncertain, and thus production of templates for nanofabrication could not advance beyond a trial-and-error stage. We present an approach combining in situ real-time grazing incidence small-angle X-ray scattering experiments (GISAXS) with model-based analysis and with ex situ atomic force microscopy (AFM) to observe this morphological transition in great detail. Our approach provides time-resolved information about all relevant morphological parameters required to trace the surface topography on the nanometer scale during reconstruction, i.e., the time dependence of the pattern wavelength, the ripple length, width, and height, and thus their facet angles. It offers a comprehensive picture of this process exemplified by a M-plane alpha-Al2O3 surface annealed at 1325 degrees C for 930 min. Fitting the model parameters to the experimental GISAXS data revealed a Johnson-Mehl-Avrami-Kolmogorov type of behavior for the pattern wavelength and a predominantly linear time dependence of the other parameters. In this case the reconstruction resulted in a crystalline surface fully patterned with asymmetric ripple-shaped nanostructures of 75 nm periodicity, 15 nm in height, and 630 nm in length. By elucidating the time dependence of these morphological parameters, this study shows a powerful way to significantly advance the predictability of annealing outcome and thus to efficiently customize nanopatterned alpha-Al2O3 templates for improved nanofabrication routines.

High-energy, ultrafast, short-wavelength infrared laser sources with high average power are important tools for industrial and scientific applications. Through the coherent combination of four ultrafast thulium-doped rod-type fiber amplifiers, we demonstrate a Tm-doped chirped pulse amplification system with a compressed pulse energy of 1.65 mJ and 167 W of average output power at a repetition rate of 101 kHz. The system delivers 85 fs pulses with a peak power of 15 GW. Additionally, the system presents a high long- and short-term stability. To the best of our knowledge, this is the highest average output power short wavelength IR, mJ-class source to date. This result shows the potential of coherent beam combining techniques in the short wavelength infrared spectral region for the power scalability of these systems.

Image plates (IPs) are a popular detector in the field of laser driven ion acceleration, owing to their high dynamic range and reusability. An absolute calibration of these detectors to laser-driven protons in the routinely produced tens of MeV energy range is, therefore, essential. In this paper, the response of Fujifilm BAS-TR IPs to 1-40 MeV protons is calibrated by employing the detectors in high resolution Thomson parabola spectrometers in conjunction with a CR-39 nuclear track detector to determine absolute proton numbers. While CR-39 was placed in front of the image plate for lower energy protons, it was placed behind the image plate for energies above 10 MeV using suitable metal filters sandwiched between the image plate and CR-39 to select specific energies. The measured response agrees well with previously reported calibrations as well as standard models of IP response, providing, for the first time, an absolute calibration over a large range of proton energies of relevance to current experiments.

Multicore fiber (MCF) amplifiers have gained increasing interest over the past years and shown their huge potential in first experiments. However, high thermal loads can be expected when operating such an amplifier at its limit. Especially in short MCF amplifiers that are pumped in counter-propagation, this leads to non-uniform mode-shrinking in the cores and, consequently, to a degradation of the system performance. In this work we show different ways to counteract the performance limitations induced by thermal effects in coherently-combined, multicore fiber amplifiers. First, we will show that pumping MCFs in co-propagation will significantly improve the combinable average power since the thermal load at the fiber end is reduced. However, this approach might not be favorable for high energy extraction. Therefore, we will introduce a new MCF design pumped in counter-propagation that leads to a reduction of the thermal load at the fiber end, which will allow for both high combined output power and pulse energy.

We report on the realization of an extremely sensitive x-ray polarization microscope, allowing to detect tiniest polarization changes of 1 in 100 billion (10(-11)) with a mu m-size focused beam. The extreme degree of polarization purity places the most stringent requirements on the orientation of the polarizer and analyzer crystals as well as the composition and the form fidelity of the lenses, which must not exhibit any birefringence. The results show that these requirements are currently only met by polymer lenses. Highly sensitive scanning x-ray polarization microscopy thus is established as a new method. It can provide new insights in a wide range of applications ranging from quantum electrodynamics and quantum optics to x-ray spectroscopy, materials research, and laser physics.

For decelerated bare lead ions at a low beam energy of 10 MeV/u, the x-ray emission associated with radiative recombination (RR) at threshold energies has been studied at the electron cooler of CRYRING@ESR at GSI, Darmstadt. In our experiment, we observed the full x-ray emission pattern by utilizing dedicated x-ray detection chambers installed at 0∘ and 180∘ observation geometry. Most remarkably, no line distortion effects due to delayed emission are present in the well-defined x-ray spectra, spanning a wide range of x-ray energies (from about 5 to 100 keV), which enables us to identify fine-structure resolved Lyman, Balmer, and Paschen x-ray lines along with the RR transitions into the K, L, and M shells of the ions. For comparison with theory, an elaborate theoretical model is established taking into account the initial population distribution via RR for all atomic levels up to Rydberg states with principal quantum number n=165 in combination with time-dependent feeding transitions. Within the statistical accuracy, the experimental data are in very good agreement with the results of rigorous relativistic predictions. Most notably, this comparison sheds light on the contribution of prompt and delayed x-ray emission (up to 70 ns) to the observed x-ray spectra, originating in particular from yrast transitions into inner shells.

Reflection ptychography is a lensfree microscopy technique particularly promising in regions of the electromagnetic spectrum where imaging optics are inefficient or not available. This is the case in tabletop extreme ultraviolet microscopy and grazing incidence small angle x ray scattering experiments. Combining such experimental configurations with ptychography requires accurate knowledge of the relative tilt between the sample and the detector in non-coplanar scattering geometries. Here, we describe an algorithm for tilt estimation in reflection ptychography. The method is verified experimentally, enabling sample tilt determination within a fraction of a degree. Furthermore, the angle-estimation uncertainty and reconstruction quality are studied for both smooth and highly structured beams.