Peer-Review Publications

The interaction of intense light with matter gives rise to competing nonlinear responses that can dynamically change material properties. Prominent examples are saturable absorption (SA) and two-photon absorption (TPA), which dynamically increase and decrease the transmission of a sample depending on pulse intensity, respectively. The availability of intense soft X-ray pulses from free-electron lasers (FELs) has led to observations of SA and TPA in separate experiments, leaving open questions about the possible interplay between and relative strength of the two phenomena. Here, we systematically study both phenomena in one experiment by exposing graphite films to soft X-ray FEL pulses of varying intensity. By applying real-time electronic structure calculations, we find that for lower intensities the nonlinear contribution to the absorption is dominated by SA attributed to ground-state depletion; our model suggests that TPA becomes more dominant for larger intensities (>1014 W/cm(2)). Our results demonstrate an approach of general utility for interpreting FEL spectroscopies.

Light carrying time-varying orbital angular momentum (OAM) is a recently discovered type of structured electromagnetic field compared with a typical vortex field whose OAM is static. Such so-called self-torqued light is employed for manipulating the fast magnetic, topological, and quantum excitations and increasing its intensity and having access to shorter pulse durations would be of great benefit. Here we theoretically and numerically demonstrate the generation of intense self-torqued harmonics and attosecond pulses in the relativistic regime, driven by two time-delayed relativistic vortex lasers with different OAMs l1 and l2. The OAM of the nth harmonic spans nl1 to nl2, and the OAM of the attosecond pulses changes from l1 to l2. Such intense self-torqued harmonics and attosecond pulses may offer alternative possibilities in ultrafast spectroscopy.

High-harmonic generation (HHG) in solids has been touted as a way to probe ultrafast dynamics and crystal symmetries in condensed matter systems. Here, we investigate the polarization properties of highorder harmonics generated in monolayer MoS2, as a function of crystal orientation relative to the midinfrared laser field polarization. At several different laser wavelengths we experimentally observe a prominent angular shift of the parallel-polarized odd harmonics for energies above approximately 3.5 eV, and our calculations indicate that this shift originates in subtle differences in the recombination dipole strengths involving multiple conduction bands. This observation is material specific and is in addition to the angular dependence imposed by the dynamical symmetry properties of the crystal interacting with the laser field, and may pave the way for probing the vectorial character of multiband recombination dipoles.

The strong-field approximation (SFA) has been widely applied in the literature to model the ionization of atoms and molecules by intense laser pulses. A recent re-formulation of the SFA in terms of partial waves and spherical tensor operators helped adopt this approach to account for realistic atomic potentials and pulses of different shape and time structure. This re-formulation also enables one to overcome certain limitations of the original SFA formulation with regard to the representation of the initial-bound and final-continuum wave functions of the emitted electrons. We here show within the framework of JAC, the Jena Atomic Calculator, how the direct SFA ionization amplitude can be readily generated and utilized in order to compute above-threshold ionization (ATI) distributions for many-electron targets and laser pulses of given frequency, intensity, polarization, pulse duration and carrier-envelope phase. Examples are shown for selected ATI energy, angular as well as momentum distributions in the strong-field ionization of atomic krypton. We also briefly discuss how this approach can be extended to incorporate rescattering and high-harmonic processes into the SFA amplitudes.

Scattering of intense laser pulses on high-energy electron beams allows one to produce a large number of x and gamma rays. For temporally pulsed lasers, the resulting spectra are broadband which severely limits practical applications. One could use linearly chirped laser pulses to compensate for that broadening. We show for laser pulses chirped in the spectral domain that there is the optimal chirp parameter at which the spectra have the brightest peak. Additionally, we use catastrophe theory to analytically find this optimal chirp value.

Many applications of two-dimensional materials such as graphene require the encapsulation in bulk material. While a variety of methods exist for the structural and functional characterization of uncovered 2D materials, there is a need for methods that image encapsulated 2D materials as well as the surrounding matter. In this work, we use extreme ultraviolet coherence tomography to image graphene flakes buried beneath 200 nm of silicon. We show that we can identify mono-, bi-, and trilayers of graphene and quantify the thickness of the silicon bulk on top by measuring the depth-resolved reflectivity. Furthermore, we estimate the quality of the graphene interface by incorporating a model that includes the interface roughness. These results are verified by atomic force microscopy and prove that extreme ultraviolet coherence tomography is a suitable tool for imaging 2D materials embedded in bulk materials.

Quantum field theory predicts that the vacuum exhibits a nonlinear response to strong electromagnetic fields. This fundamental tenet has remained experimentally challenging and is yet to be tested in the laboratory. We present proof of concept and detailed theoretical analysis of an experimental setup for precision measurements of the quantum vacuum signal generated by the collision of a brilliant x-ray probe with a high-intensity pump laser. The signal features components polarized parallel and perpendicularly to the incident x-ray probe. Our proof-of-concept measurements show that the background can be efficiently suppressed by many orders of magnitude which should not only facilitate a detection of the perpendicularly polarized component of the nonlinear vacuum response, but even make the parallel polarized component experimentally accessible for the first time. Remarkably, the angular separation of the signal from the intense x-ray probe enables precision measurements even in the presence of pump fluctuations and alignment jitter. This provides direct access to the low-energy constants governing light-by-light scattering.

In this work, we propose and verify experimentally a model that describes the concomitant influence of the beam size and optical roughness on the temporal contrast of optical pulses passing through a pulse stretcher in chirped-pulse amplification laser systems. We develop an analytical model that is capable of predicting the rising edge caused by the reflection from an optical element in a pulse stretcher, based on the power spectral density of the surface and the spatial beam profile on the surface. In an experimental campaign, we characterize the temporal contrast of a laser pulse that passed through either a folded or an unfolded stretcher design and compare these results with the analytical model. By varying the beam size for both setups, we verify that optical elements in the near- and the far-field act opposed to each with respect to the temporal contrast and that the rising edge caused by a surface benefits from a larger spatial beam size on that surface.

Two-phase flow is very important in many areas of science, engineering, and industry. Two-phase flow comprising gas and liquid phases is a common occurrence in oil and gas related industries. This study considers three flow regimes, including homogeneous, annular, and stratified regimes ranging from 5-90% of void fractions simulated via the Mont Carlo N-Particle (MCNP) Code. In the proposed model, two NaI detectors were used for recording the emitted photons of a cesium 137 source that pass through the pipe. Following that, fast Fourier transform (FFT), which aims to transfer recorded signals to frequency domain, was adopted. By analyzing signals in the frequency domain, it is possible to extract some hidden features that are not visible in the time domain analysis. Four distinctive features of registered signals, including average value, the amplitude of dominant frequency, standard deviation (STD), and skewness were extracted. These features were compared to each other to determine the best feature that can offer the best separation. Furthermore, artificial neural network (ANN) was utilized to increase the efficiency of two-phase flowmeters. Additionally, two multi-layer perceptron (MLP) neural networks were adopted for classifying the considered regimes and estimating the volumetric percentages. Applying the proposed model, the outlined flow regimes were accurately classified, resulting in volumetric percentages with a low root mean square error (RMSE) of 1.1%.

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.