Peer-Review Publications

The lack of available table-top extreme ultraviolet (XUV) sources with high enough fluxes and coherence properties has limited the availability of nonlinear XUV and x-ray spectroscopies to free-electron lasers ( FELs). Here, we demonstrate second harmonic generation (SHG) on a table-top XUV source by observing SHG near the TiM2,3 edge with a high-harmonic seeded soft x-ray laser. Furthermore, this experiment represents the first SHG experiment in the XUV. First-principles electronic structure calculations suggest the surface specificity and separate the observed signal into its resonant and nonresonant contributions. The realization of XUV-SHG on a table-top source opens up more accessible opportunities for the study of element-specific dynamics in multicomponent systems where surface, interfacial, and bulk-phase asymmetries play a driving role.

We experimentally analyze the average-power-scaling capabilities of ultrafast, thulium-doped fiber amplifiers. It has been theoretically predicted that thulium-doped fiber laser systems, with an emission wavelength around 2 mu m, should be able to withstand much higher heat-loads than their Yb-doped counterparts before the onset of transverse mode instability (TMI) is observed. In this work we experimentally verify this theoretical prediction by operating thulium doped fibers at very high heat-load. In separate experiments we analyze the performance of two different large-core, thulium-doped fiber amplifiers. The first experiment aims at operating a short, very-large core, thulium-doped fiber amplifier at extreme heat-load levels of more than 300 W/m. Even at this extreme heat-load level, the onset of TMI is not observed. The second experiment maximizes the extractable average-output power from a large-core, thulium-doped, fiber amplifier. We have achieved a pump-limited average output power of 1.15 kW without the onset of TMI. However, during a longer period of operation at this power level the amplifier performance steadily degraded and TMI could be observed for average powers in excess of 847 W thereafter. This is the first time, to the best of our knowledge, that TMI has been reported in a thulium-doped fiber amplifier.

We present an overview of recent results on optical coherence tomography with the use of extreme ultraviolet and soft X-ray radiation (XCT). XCT is a cross-sectional imaging method that has emerged as a derivative of optical coherence tomography (OCT). In contrast to OCT, which typically uses near-infrared light, XCT utilizes broad bandwidth extreme ultraviolet (XUV) and soft X-ray (SXR) radiation (Fuchs et al in Sci Rep 6:20658, 2016). As in OCT, XCT\textquotesingle s axial resolution only scales with the coherence length of the light source. Thus, an axial resolution down to the nanometer range can be achieved. This is an improvement of up to three orders of magnitude in comparison to OCT. XCT measures the reflected spectrum in a common-path interferometric setup to retrieve the axial structure of nanometer-sized samples. The technique has been demonstrated with broad bandwidth XUV/SXR radiation from synchrotron facilities and recently with compact laboratory-based laser-driven sources. Axial resolutions down to 2.2 nm have been achieved experimentally. XCT has potential applications in three-dimensional imaging of silicon-based semiconductors, lithography masks, and layered structures like XUV mirrors and solar cells.

Phonon modes play a vital role in the cooperative phenomenon of light-induced spin transitions in spin crossover (SCO) molecular complexes. Although the cooperative vibrations, which occur over several hundreds of picoseconds to nanoseconds after photoexcitation, are understood to play a crucial role in this phase transition, they have not been precisely identified. Therefore, we have performed a novel optical laser pump-nuclear resonance probe experiment to identify the Fe-projected vibrational density of states (pDOS) during the first few nanoseconds after laser excitation of the mononuclear Fe(II) SCO complex [Fe(PM-BiA)(2)(NCS)(2)]. Evaluation of the so obtained nanosecond-resolved pDOS yields an excitation of similar to 8% of the total volume of the complex from the low-spin to high-spin state. Density functional theory calculations allow simulation of the observed changes in the pDOS and thus identification of the transient inter- and intramolecular vibrational modes at nanosecond time scales.

The 2S1/2−2P1/2 and 2S1/2−2P3/2 transitions in Li-like carbon ions stored and cooled at a velocity of beta=0.47 in the experimental storage ring (ESR) at the GSI Helmholtz Centre in Darmstadt have been investigated in a laser spectroscopy experiment. Resonance wavelengths were obtained using a new continuous-wave UV laser system and a novel extreme UV (XUV) detection system to detect forward emitted fluorescence photons. The results obtained for the two transitions are compared to existing experimental and theoretical data. A discrepancy found in an earlier laser spectroscopy measurement at the ESR with results from plasma spectroscopy and interferometry has been resolved and agreement between experiment and theory is confirmed.

Quantum vacuum fluctuations give rise to effective nonlinear interactions between electromagnetic fields. A prominent signature of quantum vacuum nonlinearities driven by macroscopic fields are signal photons differing in characteristic properties such as frequency, propagation direction and polarization from the driving fields. We devise a strategy for the efficient tracing of the various vacuum-fluctuation-mediated interaction processes in order to identify the most prospective signal photon channels. As an example, we study the collision of up to four optical laser pulses and pay attention to sum and difference frequency generation. We demonstrate how this information can be used to enhance the signal photon yield in laser pulse collisions for a given total laser energy.

CThe two-photon-exchange diagrams for atoms with single valence electrons are investigated. Calculation formulas are derived for an arbitrary state within the rigorous bound-state QED framework utilizing the redefined vacuum formalism. In contrast to other methods, the redefined vacuum approach enables the identification of eight gauge-invariant subsets and, thus, efficiently checks the consistency of the obtained results. The gauge invariance of found subsets is demonstrated both analytically (for an arbitrary state) as well as numerically for 2s, 2p(1/2), and 2p(3/2) valence electrons in Li-like ions. Identifying gauge-invariant subsets in the framework of the proposed approach opens a way to tackle more complex diagrams, e.g., three-photon exchange, where the fragmentation on simpler subsets is crucial for its successful calculation.

High harmonic generation (HHG) enables coherent extreme-ultraviolet (XUV) radiation with ultra-short pulse duration in a table-top setup. This has already enabled a plethora of applications. Nearly all of these applications would benefit from a high photon flux to increase the signal-to-noise ratio and decrease measurement times. In addition, shortest pulses are desired to investigate fastest dynamics in fields as diverse as physics, biology, chemistry and material sciences. In this work, the up-to-date most powerful table-top XUV source with 12.9 ± 3.9 mW in a single harmonic line at 26.5 eV is demonstrated via HHG of a frequency-doubled and post-compressed fibre laser. At the same time the spectrum supports a Fourier-limited pulse duration of sub-6 fs in the XUV, which allows accessing ultrafast dynamics with an order of magnitude higher photon flux than previously demonstrated. This concept will greatly advance and facilitate applications of XUV radiation in science and technology and enable photon-hungry ultrafast studies.

An ultrafast fiber chirped-pulse amplification laser system based on a coherent combination of 16 ytterbium-doped rod-type amplifiers is presented. It generates 10 mJ pulse energy at 1 kW average power and 120 fs pulse duration. A partially helium-protected, two-staged chirped-pulse amplification grating compressor is implemented to maintain the close to diffraction-limited beam quality by avoiding nonlinear absorption in air. (C) 2021 Optical Society of America under the terms of the OSA Open Access Publishing Agreement

Atomic cascades are ubiquitous in nature and they have been explored within very different scenarios, from precision measurements to the modeling of astrophysical spectra, and up to the radiation damage in biological matter. However, up to the present, a quantitative analysis of these cascades often failed because of their inherent complexity. Apart from utilizing the rotational symmetry of atoms and a proper distinction of different physical schemes, a hierarchy of useful approaches is therefore needed in order to keep cascade computations feasible. We here suggest a classification of atomic cascades and demonstrate how they can be modeled within the framework of the Jena Atomic Calculator. As an example, we shall compute within a configuration-average approach the stepwise decay cascade of atomic magnesium, following a 1s inner-shell ionization, and simulate the corresponding (final) ion distribution. Our classification of physical scenarios (schemes) and the hierarchy of computational approaches are both flexible to further refinements as well as to complex shell structures of the atoms and ions, for which the excitation and decay dynamics need to be modeled in good detail.

We present a diode-pumped, electro-optically Q-switched Tm:YAG laser with a cryogenically cooled laser crystal at 120 K. Output pulses of up to 2.55 mJ and 650 ns duration were demonstrated in an actively Q-switched configuration with a repetition rate of 1 Hz. By using cavity dumping the pulse duration was shortened to 18 ns with only a slightly lower output energy of 2.22 mJ. Furthermore, using a simplified rate equation model, we discuss design constraints on the pump fluence in a pulse pump approach for Tm:YAG to maximize the energy storage capability at a given pump power.

We theoretically study frustrated double ionization (FDI) of atoms subjected to intense circularly polarized laser pulses using a three-dimensional classical model. We find a \textasciigrave knee\textquotesingle structure of FDI probability as a function of intensity, which is similar to the intensity dependence of nonsequential double ionization probability. The observation of FDI is more favourable when using targets with low ionization potentials and short driving laser wavelengths. This is attributed to the crucial role of recollision therein, which can be experimentally inferred from the photoelectron momentum distribution generated by FDI. This work provides novel physical insights into FDI dynamics with circular polarization.

Above-threshold ionization spectra from cesium are measured as a function of the carrier-envelope phase (CEP) using laser pulses centered at 3.1  μm wavelength. The directional asymmetry in the energy spectra of backscattered electrons oscillates three times, rather than once, as the CEP is changed from 0 to 2π. Using the improved strong-field approximation, we show that the unusual behavior arises from the interference of few quantum orbits. We discuss the conditions for observing the high-order CEP dependence, and draw an analogy with time-domain holography with electron wave packets.

In this study, we examine the quality of microscale ghost images as a function of the measured histographic signal distribution of the speckle fields from a nonuniform pseudothermal light source. This research shows that the distribution of the detected signal level on each pixel of the camera plays a significant role in improving the contrast-to-noise ratio (CNR) of pseudothermal ghost imaging. To our knowledge, the scaling of CNR with different pixel intensity distributions of the speckle fields is observed for the first time in the field of pseudothermal microscale ghost imaging. The experimental observations are in very good agreement with numerical analysis. Based on these findings, we can predict the settings for light sources that will maximize the CNR of microscale ghost images.

Differentially pumped capillaries, i.e., capillaries operated in a pressure gradient environment, are widely used for nonlinear pulse compression. In this work, we show that strong pressure gradients and high gas throughputs can cause spatiotemporal instabilities of the output beam profile. The instabilities occur with a sudden onset as the flow evolves from laminar to turbulent. Based on the experimental and numerical results, we derive guidelines to predict the onset of those instabilities and discuss possible applications in the context of nonlinear flow dynamics. (C) 2021 Optical Society of America under the terms of the OSA Open Access Publishing Agreement

Many applications ranging from nonlinear optics to material processing would benefit from pulsed ultrashort (quasi-)non-diffracting Gauss-Bessel beams (GBBs). Here we demonstrate a straightforward yet efficient method for generating such zeroth- and first-order GBBs using a single reflective spatial light modulator. Even in the sub-8-fs range there are no noticeable consequences for the measured pulse duration. The only effect is a weak coloring of the outer-lying satellite rings of the beams due to the spectrum spanning over more than 300 nm. The obtained beams have diffraction half-angles below 40 mu rad and reach propagation distances in excess of 1.5 m.

In this manuscript we demonstrate a method to reconstruct the wavefront of focused beams from a measured diffraction pattern behind a diffracting mask in real-time. The phase problem is solved by means of a neural network, which is trained with simulated data and verified with experimental data. The neural network allows live reconstructions within a few milliseconds, which previously with iterative phase retrieval took several seconds, thus allowing the adjustment of complex systems and correction by adaptive optics in real time. The neural network additionally outperforms iterative phase retrieval with high noise diffraction patterns.

A combined experimental and theoretical study on single capture in 15–50keV/uC4+ + He collisions was performed. State-selective single-electron capture cross sections and projectile scattering angle distributions were obtained by using a reaction microscope. A comparison of the state-selective cross sections with theoretical calculations based on the two-active-electron semiclassical atomic-orbital close-coupling method showed an excellent agreement for the considered impact energies. For the angular differential cross sections, an overall agreement was also obtained between the present experimental and theoretical results. Simulations performed using an extended Fraunhofer-type diffraction model suggest that the undulatory structures observed at small scattering angles for capture to C3+(1s22s) and C3+(1s22p0) can be interpreted as the diffraction pattern of the incident projectile de Broglie wave confined by an aperture defined as the region around the target where the considered capture process is likely. The strong competition between single-electron capture to C3+(1s22p0) and C3+(1s22p1) is also discussed to interpret the differences observed between their respective differential cross sections.

Non-destructive measurements of nA beam currents in particle beam storage rings by detecting the azimuthal magnetic field generated by moving charged particles with a Cryogenic Current Comparator (CCC) are well established. The detection of beam currents with small amplitudes with a CCC in a storage ring demands a high slew rate which is caused by the rapid change of the beam current exceeding the operational limit of the SQUID in flux-locked loop mode. Previous solutions to increase the slew rate used a LCR first-order low-pass filter were a small resistor, unfortunately, dominated the current noise of the CCC. In this work we present a novel take by adding a second resonator into the CCC which in turn allows for higher resistances of the LCR low-pass filter and therefore lower thermal current noise. A second challenge connected with this CCC approach is the residual magnetization of the highly permeable magnetic core and the resulting shielding currents in the superconducting circuits of the CCC. The timing of a storage ring in the range of minutes opens a way to reduce these DC currents using a LR high-pass filter. Using serial sub-micro ohm resistors, time constants in the hour range can be achieved to improve the stability and performance of the CCC system.

Bright, coherent soft X-ray radiation is essential to a variety of applications in fundamental research and life sciences. To date, a high photon flux in this spectral region can only be delivered by synchrotrons, free-electron lasers or high-order harmonic generation sources, which are driven by kHz-class repetition rate lasers with very high peak powers. Here, we establish a novel route toward powerful and easy-to-use SXR sources by presenting a compact experiment in which nonlinear pulse self-compression to the few-cycle regime is combined with phase-matched high-order harmonic generation in a single, helium-filled antiresonant hollow-core fibre. This enables the first 100 kHz-class repetition rate, table-top soft X-ray source that delivers an application-relevant flux of 2.8 x 10(6) photon s(-1) eV(-1) around 300 eV. The fibre integration of temporal pulse self-compression (leading to the formation of the necessary strong-field waveforms) and pressure-controlled phase matching will allow compact, high-repetition-rate laser technology, including commercially available systems, to drive simple and cost-effective, coherent high-flux soft X-ray sources.

The 35-fs-long pulses of a commercial Ti:sapphire amplifier are compressed to similar to 20 fs via self-phase modulation in bulk glass substrates. The cascading of both nonlinear broadening and dispersion compensation stages makes use of the increasing peak power in the successive nonlinear stages. As an application example, the compressed pulses are used for electro-optical sampling of terahertz waves created by optically pumped thin-film spin emitters. (C) 2021 Optical Society of America under the terms of the OSA Open Access Publishing Agreement

Coherent control of quantum dynamics is key to a multitude of fundamental studies and applications1. In the visible or longer-wavelength domains, near-resonant light fields have become the primary tool with which to control electron dynamics2. Recently, coherent control in the extreme-ultraviolet range was demonstrated3, with a few-attosecond temporal resolution of the phase control. At hard-X-ray energies (above 5—10 kiloelectronvolts), Mössbauer nuclei feature narrow nuclear resonances due to their recoilless absorption and emission of light, and spectroscopy of these resonances is widely used to study the magnetic, structural and dynamical properties of matter4,5. It has been shown that the power and scope of Mössbauer spectroscopy can be greatly improved using various control techniques6—16. However, coherent control of atomic nuclei using suitably shaped near-resonant X-ray fields remains an open challenge. Here we demonstrate such control, and use the tunable phase between two X-ray pulses to switch the nuclear exciton dynamics between coherent enhanced excitation and coherent enhanced emission. We present a method of shaping single pulses delivered by state-of-the-art X-ray facilities into tunable double pulses, and demonstrate a temporal stability of the phase control on the few-zeptosecond timescale. Our results unlock coherent optical control for nuclei, and pave the way for nuclear Ramsey spectroscopy17 and spin-echo-like techniques, which should not only advance nuclear quantum optics18, but also help to realize X-ray clocks and frequency standards19. In the long term, we envision time-resolved studies of nuclear out-of-equilibrium dynamics, which is a long-standing challenge in Mössbauer science20.

Relative narrow bandwidth-high energy radiation can be produced through Thomson scattering, where highly relativistic electrons collide with a laser pulse. The bandwidth of such a source is determined, among others factors, by the bandwidth of the laser pulse and the energy spread of the electrons. Here we investigate how the bandwidth of such a source can be minimized, with a particular emphasis on electron bunches with a correlated energy spread of several percent, that are typical for plasma based accelerator schemes. We show that by introducing a chirp on the laser pulse it is possible to compensate the broadening effect due to the energy spread of the electrons, and obtain the same bandwidth as a quasi-monochromatic plane wave laser pulse colliding with a monoenergetic electron bunch. Ultimately, the bandwidth of a Thomson source is limited by the acceptance angle and the initial transverse momentum of electrons (emittance).

Bessel beams are remarkable since they do not diverge. Accordingly, they have numerous applications ranging from precision laser micro-machining to laser particle acceleration. We demonstrate a novel approach for generating long-range Gauss-Bessel beams. A ring-shaped beam is produced by imprinting a vortex with high topological charge in a Gaussian beam. The phase singularities are thereafter removed and the ring-shaped beam focused/Fourier-transformed by a thin lens. This results in a remarkably good realization of a Gauss- Bessel beam. Divergence angles in the microradian range and Gauss-Bessel beam lengths up to 2.5 m behind the focal plane of the lens are demonstrated.

Scientific and technological progress depend substantially on the ability to image on the nanoscale. In order to investigate complex, functional, nanoscopic structures like, e.g., semiconductor devices, multilayer optics, or stacks of 2D materials, the imaging techniques not only have to provide images but should also provide quantitative information. We report the material-specific characterization of nanoscopic buried structures with extreme ultraviolet coherence tomography. The method is demonstrated at a laser-driven broadband extreme ultraviolet radiation source, based on high-harmonic generation. We show that, besides nanoscopic axial resolution, the spectral reflectivity of all layers in a sample can be obtained using algorithmic phase reconstruction. This provides localized, spectroscopic, material-specific information of the sample. The method can be applied in, e.g., semiconductor production, lithographic mask inspection, or quality control of multilayer fabrication. Moreover, it paves the way for the investigation of ultrafast nanoscopic effects at functional buried interfaces. Published by The Optical Society under the terms of the Creative Commons Attribution 4.0 License.