Peer-Review Publications

Be-like ¹³⁶Xe⁵⁰⁺ ions have been investigated employing the resonant electron-ion collision process of dielectronic recombination (DR) as a spectroscopic tool. The experiments were performed at the experimental storage ring in Darmstadt, Germany, using its electron cooler as a target for free electrons. DR Rydberg resonance series 2s²+e⁻ \to 2s 2pj n lj for the associated intra-L-shell transitions 2s² ¹S₀ - 2s 2p₁/₂ ³P₁, 2s² ¹S₀ - 2s 2p₃/₂ ³P₂ and 2s² ¹S₀ - 2s 2p₃/₂ ¹P₁ were observed with high resolution. In addition to these excitations from the ground state we determined resonances associated with excitations 2s 2p₁/₂ ³P₀ to 2p₁/₂ 2p₃/₂ ³P₁ of ions initially in the metastable 2s 2p₁/₂ ³P₀ state. The corresponding excitation energies were determined to be E(¹S₀ \to ³P₁)=127.269(46) eV, E(¹S₀ \to ³P₂)=469.474(81) eV and E(¹S₀ to ¹P₁)=532.801(16) eV and E(³P₀ to 2p₁/₂ 2p₃/₂ ³P₁)=533.733(22) eV. These excitation energies are compared with previous measurements and with recent state-of-the-art atomic structure calculations.

Triple photoionization of Xe³⁺, Xe⁴⁺ and Xe⁵⁺ ions has been studied in the energy range 670-750 eV, including the 3d ionization threshold. The photon-ion merged-beam technique was used at a synchrotron light source to measure the absolute photoionization cross sections. These cross sections exhibit a progressively larger number of sharp resonances as the ion charge state is increased. This clearly visualizes the re-ordering of the ε f continuum into a regular series of (bound) Rydberg orbitals as the ionic core becomes more attractive. The energies and strengths of the resonances are extracted from the experimental data and are further analysed by relativistic atomic-structure calculations.

We present measurements of the complex ion structure of warm dense carbon close to the melting line at pressures around 100 GPa. High-pressure samples were created by laser-driven shock compression of graphite and probed by intense laser-generated x-ray sources with photon energies of 4.75 keV and 4.95 keV. High-efficiency crystal spectrometers allow for spectrally resolving the scattered radiation. Comparing the ratio of elastically and inelastically scattered radiation, we find evidence for a complex bonded liquid that is predicted by ab-initio quantum simulations showing the influence of chemical bonds under these conditions. Using graphite samples of different initial densities we demonstrate the capability of spectrally resolved x-ray scattering to monitor the carbon solid-liquid transition at relatively constant pressure of 150 GPa. Showing first single-pulse scattering spectra from cold graphite of unprecedented quality recorded at the Linac Coherent Light Source, we demonstrate the outstanding possibilities for future high-precision measurements at 4th Generation Light Sources.

Group velocity control is demonstrated for x-ray photons of 14.4 keV energy via a direct measurement of the temporal delay imposed on spectrally narrow x-ray pulses. Subluminal light propagation is achieved by inducing a steep positive linear dispersion in the optical response of Fe57 Mössbauer nuclei embedded in a thin film planar x-ray cavity. The direct detection of the temporal pulse delay is enabled by generating frequency-tunable spectrally narrow x-ray pulses from broadband pulsed synchrotron radiation. Our theoretical model is in good agreement with the experimental data.

We present recent advances in the development of atomic ab initio multiconfiguration Dirac-Hartree-Fock theory, implemented in the GRASP relativistic atomic structure code. For neutral atoms, the deviations of properties calculated within the Dirac-Hartree-Fock (DHF) method (based on independent particle model of an atomic cloud) are usually dominated by electron correlation effects, i.e. the non-central interactions of individual electrons. We present the recent advances in accurate calculations of electron correlation effects in small, medium, and heavy neutral atoms. We describe methods of systematic development of multiconfiguration expansions leading to systematic, controlled improvement of the accuracy of the ab initio calculations. These methods originate from the concept of the complete active space (CAS) model within the DHF theory, which, at least in principle, permits fully relativistic calculations with full account of electron correlation effects. The calculations within the CAS model on currently available computer systems are feasible only for very light systems. For heavier atoms or ions with more than a few electrons, restrictions have to be imposed on the multiconfiguration expansions. We present methods and tools, which are designed to extend the numerical calculations in a controlled manner, where multiconfiguration expansions account for all leading electron correlation effects. We show examples of applications of the GRASP code to calculations of hyperfine structure constants, but the code may be used for calculations of arbitrary bound-state atomic properties. In recent years it has been applied to calculations of atomic and ionic spectra (transition energies and rates), to determinations of nuclear electromagnetic moments, as well as to calculations related to interactions of bound electrons with nuclear electromagnetic moments leading to violations of discrete symmetries.

Crystalline Au nanoparticles embedded in epitaxially grown SrTiO₃ layers were prepared by an annealing and coating procedure of Au seed layers on SrTiO₃ (STO) substrates. X-ray diffraction and transmission electron microscopy measurements were performed to investigate the size, shape, and deformation of the particles and their crystal orientation. The shape and size of the crystalline Au nanoparticles can be tuned by controlling the Au seed layer thickness and single crystalline elliptically shaped Au nanoparticles have been generated. Furthermore, the orientation of the surrounding SrTiO₃ matrix changes significantly from homoepitaxially grown (001) to secondary (111) and (011) orientations for Au seed layers that are thicker than 4 nm. This is of great interest for modifying the electrical properties of SrTiO₃ layers, whereas the anisotropically shaped crystalline particles are relevant for optical applications, due to localized surface plasmon resonances.

The process of high harmonic generation (HHG) enables the development of table-top sources of coherent extreme ultraviolet (XUV) light. Although these are now matured sources, they still mostly rely on bulk laser technology that limits the attainable repetition rate to the low kilohertz regime. Moreover, many of the emerging applications of such light sources (e.g., photoelectron spectroscopy and microscopy, coherent diffractive imaging, or frequency metrology in the XUV spectral region) require an increase in the repetition rate. Ideally, these sources are operated with a multi-MHz repetition rate and deliver a high photon flux simultaneously. So far, this regime has been solely addressed using passive enhancement cavities together with low energy and high repetition rate lasers. Here, a novel route with significantly reduced complexity (omitting the requirement of an external actively stabilized resonator) is demonstrated that achieves the previously mentioned demanding parameters. A krypton-filled Kagome photonic crystal fiber is used for efficient nonlinear compression of 9 mJ, 250 fs pulses leading to ,7 mJ, 31 fs pulses at 10.7 MHz repetition rate. The compressed pulses are used for HHG in a gas jet. Particular attention is devoted to achieving phase-matched (transiently) generation yielding .10^13 photons s-1 (.50 mW) at 27.7 eV. This new spatially coherent XUV source improved the photon flux by four orders of magnitude for direct multi-MHZ experiments, thus demonstrating the considerable potential of this source.

We present two Penning trap experiments concerned with different aspects of the physics of extreme electromagnetic fields, the ARTEMIS experiment designed for bound-electron magnetic moment measurements in the presence of the extremely strong fields close to the nucleus of highly charged ions, and the HILITE experiment, in which well-defined ion targets are to be subjected to high-intensity laser fields.

The linear polarization of x rays produced by dielectronic recombination into highly charged xenon ions was measured at an electron beam ion trap using the Compton polarimetry technique. This opens numerous possibilities for diagnostics of anisotropies of hot plasmas. Moreover, it was observed that the polarization of x rays, following the dielectronic capture populating the [1s 2s2 2p1/2]_1 state, is highly sensitive to the Breit interaction. The experimental results for this transition rule out by 5σ calculations not taking the Breit interaction into account.

Starting from the Heisenberg-Euler effective Lagrangian, we determine the photon current and photon polarization tensor in inhomogeneous, slowly varying electromagnetic fields. To this end, we consider background field configurations varying in both space and time, paying special attention to the tensor structure. As a main result, we obtain compact analytical expressions for the photon polarization tensor in realistic Gaussian laser pulses, as generated in the focal spots of high-intensity lasers. These expressions are of utmost importance for the investigation of quantum vacuum nonlinearities in realistic high-intensity laser experiments.

An undulator is proposed based on the plasma wakefields excited by a laser pulse in a plasma channel. Generation of the undulator fields is achieved by inducing centroid oscillations of the laser pulse in the channel. The period of such an undulator is proportional to the Rayleigh length of the laser pulse and can be submillimeter, while preserving high undulator strength. The electron trajectories in the undulator are examined, expressions for the undulator strength are presented, and the spontaneous radiation is calculated. Multimode and multicolor laser pulses are considered for greater tunability of the undulator period and strength.

We reconsider the recently proposed nonlinear quantum electrodynamics effect of quantum reflection of photons off an inhomogeneous strong-field region. We present new results for strong fields varying both in space and time. While such configurations can give rise to new effects such as frequency mixing, estimated reflection rates based on previous one-dimensional studies are corroborated. On a conceptual level, we critically re-examine the validity regime of the conventional locally-constant-field approximation and identify kinematic configurations which can be treated reliably. Our results further underline the discovery potential of quantum reflection as a new signature of the nonlinearity of the quantum vacuum.

Relativistic configuration-interaction calculations have been performed for energy levels of the low-lying and core-excited states of beryllium-like argon, Ar14+. These calculations include the one-loop quantum electrodynamics (QED) effects as obtained by two different methods: the screening-potential approach and the model QED operator approach. The calculations are supplemented by a systematic estimation of the uncertainties of the theoretical predictions.

The radiative capture of free electrons (radiative recombination) and bound electrons (radiative electron capture) are among the most important charge changing processes for fast, highly-charged ions. While total cross sections can be obtained by an approximate formula with reasonable accuracy, the estimation of angular distributions and polarization properties of the emitted radiation requires a fully relativistic treatment that is numerical expensive. Therefore we recently started the development of a fast calculator for these radiation characteristics. The program is based on a grid of rigorously calculated data points for free- electron capture into bare ions, between which interpolation is performed to obtain radiation characteristics for specific collision systems. Also capture into few-electron systems is taken into account in an approximate way. We present first results from this development.

Self-organized monocrystalline Au nanoparticles with potential applications in plasmonics are grown in a SrTiO3 matrix by a novel two-step deposition process. The crystalline preferred orientation of these Au nanoparticles is investigated by synchrotron hard x-ray diffraction. Nanoparticles preferentially align with the (111) direction along the substrate normal (001), whereas two in-plane orientations are found with [110]SrTiO3∥[110]Au and [100]SrTiO3∥[110]Au. Additionally, a smaller diffraction signal from nanoparticles with the (001) direction parallel to the substrate normal (001) is observed; once again, two in-plane orientations are found, with [100]SrTiO3∥[100]Au and [100]SrTiO3∥[110]Au. The populations of the two in-plane orientations are found to depend on the thickness of the gold film deposited in the first step of the growth.

A method for calculations of electron-positron pair-creation probabilities in low-energy heavy-ion collisions is developed. The approach is based on the propagation of all one-electron states via the numerical solving of the time-dependent Dirac equation in the monopole approximation. The electron wave functions are represented as finite sums of basis functions constructed from B-splines using the dual-kinetic-balance technique. The calculations of the created particle numbers and the positron energy spectra are performed for the collisions of bare nuclei at the energies near the Coulomb barrier with the Rutherford trajectory and for different values of the nuclear charge and the impact parameter. To examine the role of the spontaneous pair creation, the collisions with a modified velocity and with a time delay are also considered. The obtained results are compared with the previous calculations and the possibility of observation of the spontaneous pair creation is discussed.

We study synchrotron radiation emission from laser interaction with near critical density (NCD) plasmas at intensities of 10²¹ W/cm² using three-dimensional particle-in-cell simulations. It is found that the electron dynamics depend on the laser shaping process in NCD plasmas, and thus the angular distribution of the emitted photons changes as the laser pulse evolves in space and time. The final properties of the resulting synchrotron radiation, such as its overall energy, the critical photon energy, and the radiation angular distribution, are strongly affected by the laser polarization and plasma density. By using a 420 TW/50 fs laser pulse at the optimal plasma density (~1 nc), about 10⁸ photons/0.1% bandwidth are produced at multi-MeV photon energies, providing a route to ultraintense, femtosecond gamma ray pulses.

An excited metastable nuclear state of Os192 in a hydrogen-like charge state has been studied for the first time. It was populated in projectile fragmentation of a Au197 beam on a Be9 target with the UNILAC-SIS accelerators at GSI. Fragmentation products in the region of interest were passed through the fragment separator and injected into the experimental storage ring (ESR). Cooling of the injected beam particles enabled Schottky mass spectrometry to be performed. Analysis shows the lifetime of the state to be considerably longer than that of the neutral ion [t_neut=8.5(14)s]; this change is attributed to hindrance of internal conversion in hydrogen-like Os192. Calculations have been performed to estimate the lifetime, and the result has been compared with that measured experimentally. There is good agreement between the expected [t_H-like=13.0(24)s] and measured lifetimes (t_rest=15.1+1.5-1.3 s) from the internal decay of Os192m. This provides a test for the reliability of the values obtained from internal conversion coefficient calculations in highly ionized systems and is the first measurement of its kind to be performed using the ESR setup.

We present a momentum-resolved study of strong field multiple ionization of ionic targets. Using a deconvolution method we are able to reconstruct the electron momenta from the ion momentum distributions after multiple ionization up to four sequential ionization steps. This technique allows an accurate determination of the saturation intensity as well as of the electron release times during the laser pulse. The measured results are discussed in comparison to typically used models of over-the-barrier ionization and tunnel ionization.

Narrowband x- and γ-ray sources based on the inverse Compton scattering of laser pulses suffer from a limitation of the allowed laser intensity due to the onset of nonlinear effects that increase their bandwidth. It has been suggested that laser pulses with a suitable frequency modulation could compensate this ponderomotive broadening and reduce the bandwidth of the spectral lines, which would allow one to operate narrowband Compton sources in the high-intensity regime. In this paper we therefore present the theory of nonlinear Compton scattering in a frequency-modulated intense laser pulse. We systematically derive the optimal frequency modulation of the laser pulse from the scattering matrix element of nonlinear Compton scattering, taking into account the electron spin and recoil. We show that, for some particular scattering angle, an optimized frequency modulation completely cancels the ponderomotive broadening for all harmonics of the backscattered light. We also explore how sensitively this compensation depends on the electron-beam energy spread and emittance, as well as the laser focusing.

A new generation of diode-pumped high-energy-class solid-state laser facilities is in development that generate multijoule pulse energies at around 10 Hz. Currently deployed quasi-continuous-wave (QCW) diode lasers deliver average inpulse pump powers of around 300 W per bar. Increased power-per-bar helps to reduce the system size, complexity and cost per Joule and the increased pump brilliance also enables more efficient operation of the solid state laser itself. It has been shown in recent studies, that optimized QCW diode laser bars centered at 940…980 nm can operate with an average in-pulse power of >1000 W per bar, triple that of commercial sources. When operated at pulsed condition of 1 ms, 10 Hz, this corresponds to >1 J/bar. We review here the status of these high-energy-class pump sources, showing how the highest powers are enabled by using long resonators (4…6 mm) for improved cooling and robustly passivated output facets for high reliability. Results are presented for prototype passively-cooled single bar assemblies and monolithic stacked QCW arrays. We confirm that 1 J/bar is sustained for fast-axis collimated stacks with a bar pitch of 1.7 mm, with narrow lateral far field angle (<12° with 95% power) and spectral width (<12 nm with 95% power). Such stacks are anticipated to enable Joule/bar pump densities to be used near-term in commercial high power diode laser systems. Finally, we briefly summarize the latest status of research into bars with higher efficiencies, including studies into operation at sub-zero temperatures (-70°C), which also enables higher powers and narrower far field and spectra.

In this work the latest progress in the understanding of mode instabilities is reviewed. Particular emphasis is put on the recently established influence of photodarkening on the mode instability threshold and its behavior. It is shown, for example, that even degradations of the output power in the order of a few percent can lead to very significant reductions of the mode instability threshold. Moreover, our analysis shows that photodarkening also alters the expected behavior of the mode instability threshold with respect to the signal wavelength and the seed power. Thus photodarkening is revealed as one of the main effects shaping the behavior of the mode instability threshold observed in experiments.

A way to increase the efficiency of Thulium-doped fiber systems and simultaneously prevent the generation of heat by pumping the excited state around 1460 nm has been recently proposed by the authors. In this contribution we show that a Thulium-doped fiber amplifier can lase around 1460nm while simultaneously amplifying signals around 2 μm. Such an operation results in considerably higher amplification efficiencies and in lower operating temperatures without the need for an external pump around 1460 nm.

We present characterizations of the attosecond pulse train produced in the high harmonic generation (HHG) from SF6 molecules irradiated by a strong pulsed laser field at 800 nm. At harmonic order 17, we observe a minimum in the amplitude of the emitted spectrum and a corresponding distortion in the phase. Our experimental results are compared to two models: a multicenter interference model focused on the effect of the structure of the SF6 molecule in HHG and a model focused on the interferences between multiple ionization channels in HHG. We find that the experimental results agree very well with the multiple ionization channels model, illustrating that HHG in molecules can be very complex and that it provides insights of the intramolecular electron dynamics during the interaction process.

Thulium-based fiber lasers potentially provide for the demand of high average-power ultrafast laser systems operating at an emission wavelength around 2 μm. In this work we use a Tm-doped photonic-crystal fiber (PCF) with a mode field diameter of 36 μm enabling high peak powers without the onset of detrimental nonlinear effects. For the first time a Tm-doped PCF amplifier allows for a pump-power limited average output power of 241 W with a slope efficiency above 50%, good beam quality and linear polarization. A record compressed average power of 152 W and a pulse peak power of more than 4 MW at sub-700 fs pulse duration are enabled by dielectric gratings with diffraction efficiencies higher than 98% leading to a total compression efficiency of more than 70%. A further increase of pulse peak power towards the GW-level is planned by employing Tm-doped large-pitch fibers with mode field diameters well above 50 μm. The coherent combination of ultrafast pulses might eventually lead to kW-level average power and multi-GW peak power.