Magnetic-Field Effect as a Tool to Investigate Electron Correlation in Strong-Field Ionization.

The influence of the magnetic component of the driving electromagnetic field is often neglected when investigating light-matter interaction. We show that the magnetic component of the light field plays an important role in nonsequential double ionization, which serves as a powerful tool to investigate electron correlation. We investigate the magnetic-field effects in double ionization of xenon atoms driven by near-infrared ultrashort femtosecond laser pulses and find that the mean forward shift of the electron momentum distribution in light-propagation direction agrees well with the classical prediction, where no under-barrier or recollisional nondipole enhancement is observed. By extending classical trajectory Monte Carlo simulations beyond the dipole approximation, we reveal that double ionization proceeds via recollision-induced doubly excited states, followed by subsequent sequential over-barrier field ionization of the two electrons. In agreement with this model, the binding energies do not lead to an additional nondipole forward shift of the electrons. Our findings provide a new method to study electron correlation by exploiting the effect of the magnetic component of the electromagnetic field.

Magnetic-Field Effect in High-Order Above-Threshold Ionization.

We experimentally and theoretically investigate the influence of the magnetic component of an electromagnetic field on high-order above-threshold ionization of xenon atoms driven by ultrashort femtosecond laser pulses. The nondipole shift of the electron momentum distribution along the light-propagation direction for high energy electrons beyond the 2U_{p} classical cutoff is found to be vastly different from that below this cutoff, where U_{p} is the ponderomotive potential of the driving laser field. A local minimum structure in the momentum dependence of the nondipole shift above the cutoff is identified for the first time. With the help of classical and quantum-orbit analysis, we show that large-angle rescattering of the electrons strongly alters the partitioning of the photon momentum between electron and ion. The sensitivity of the observed nondipole shift to the electronic structure of the target atom is confirmed by three-dimensional time-dependent Schrödinger equation simulations for different model potentials. Our work paves the way toward understanding the physics of extreme light-matter interactions at long wavelengths and high electron kinetic energies.

A new route for enantio-sensitive structure determination by photoelectron scattering on molecules in the gas phase.

X-Ray as well as electron diffraction are powerful tools for structure determination of molecules. Studies on randomly oriented molecules in the gas phase address cases in which molecular crystals cannot be generated or the interaction-free molecular structure is to be addressed. Such studies usually yield partial geometrical information, such as interatomic distances. Here, we present a complementary approach, which allows obtaining insight into the structure, handedness, and even detailed geometrical features of molecules in the gas phase. Our approach combines Coulomb explosion imaging, the information that is encoded in the molecular-frame diffraction pattern of core-shell photoelectrons and ab initio computations. Using a loop-like analysis scheme, we are able to deduce specific molecular coordinates with sensitivity even to the handedness of chiral molecules and the positions of individual atoms, e.g., protons.

Supercontinuum generation in a carbon disulfide core microstructured optical fiber.

We demonstrate supercontinuum generation in a liquid-core microstructured optical fiber using carbon disulfide as the core material. The fiber provides a specific dispersion landscape with a zero-dispersion wavelength approaching the telecommunication domain where the corresponding capillary-type counterpart shows unsuitable dispersion properties for soliton fission. The experiments were conducted using two pump lasers with different pulse duration (30 fs and 90 fs) giving rise to different non-instantaneous contributions of carbon disulfide in each case. The presented results demonstrate an extraordinary high conversion efficiency from pump to soliton and to dispersive wave, overall defining a platform that enables studying the impact of non-instantaneous responses on ultrafast soliton dynamics and coherence using straightforward pump lasers and diagnostics.

Double Core-Hole Generation in O_{2} Molecules Using an X-Ray Free-Electron Laser: Molecular-Frame Photoelectron Angular Distributions.

We report on a multiparticle coincidence experiment performed at the European X-ray Free-Electron Laser at the Small Quantum Systems instrument using a COLTRIMS reaction microscope. By measuring two ions and two electrons in coincidence, we investigate double core-hole generation in O_{2} molecules in the gas phase. Single-site and two-site double core holes have been identified and their molecular-frame electron angular distributions have been obtained for a breakup of the oxygen molecule into two doubly charged ions. The measured distributions are compared to results of calculations performed within the frozen- and relaxed-core Hartree-Fock approximations.

Approximate model for analyzing band structures of single-ring hollow-core anti-resonant fibers.

Precise knowledge of modal behavior is of essential importance for understanding light guidance, particularly in hollow-core fibers. Here we present a semi-analytical model that allows determination of bands formed in revolver-type anti-resonant hollow-core fibers. The approach is independent of the actual arrangement of the anti-resonant elements, does not enforce artificial lattice arrangements and allows determination of the effective indices of modes of preselected order. The simulations show two classes of modes: (i) low-order modes exhibiting effective indices with moderate slopes and (ii) a high number of high-order modes with very strong effective index dispersion, forming a quasi-continuum of modes. It is shown that the mode density scales with the square of the normalized frequency, being to some extent similar to the behavior of multimode fibers.

Link between Photoelectron Circular Dichroism and Fragmentation Channel in Strong Field Ionization.

The investigation of the photoelectron circular dichroism (PECD) in the strong field regime (800 nm, 6.9 × 1013 W/cm2) on methyloxirane (MOX) reveals a flip of the sign of PECD between different fragmentation channels. This finding is of great importance for future experiments and applications in chemistry or pharmacy using PECD in the strong field regime as analysis method. We suggest that the observed sign change of PECD is not caused by ionization from different orbitals but by effectively selecting differently oriented nonisotropic subsamples of molecules via the fragmentation channel.

Imaging the He2 quantum halo state using a free electron laser.

Quantum tunneling is a ubiquitous phenomenon in nature and crucial for many technological applications. It allows quantum particles to reach regions in space which are energetically not accessible according to classical mechanics. In this "tunneling region," the particle density is known to decay exponentially. This behavior is universal across all energy scales from nuclear physics to chemistry and solid state systems. Although typically only a small fraction of a particle wavefunction extends into the tunneling region, we present here an extreme quantum system: a gigantic molecule consisting of two helium atoms, with an 80% probability that its two nuclei will be found in this classical forbidden region. This circumstance allows us to directly image the exponentially decaying density of a tunneling particle, which we achieved for over two orders of magnitude. Imaging a tunneling particle shows one of the few features of our world that is truly universal: the probability to find one of the constituents of bound matter far away is never zero but decreases exponentially. The results were obtained by Coulomb explosion imaging using a free electron laser and furthermore yielded He2's binding energy of [Formula: see text] neV, which is in agreement with most recent calculations.

Polarization evolution in single-ring antiresonant hollow-core fibers.

Understanding polarization in waveguides is of fundamental importance for any photonic device and is particularly relevant within the scope of fiber optics. Here, we investigate the dependence of the geometry-induced polarization behavior of single-ring antiresonant hollow-core fibers on various parameters from the experimental perspective, showing that structural deviations from an ideal polygonal shape impose birefringence and polarization-dependent loss, confirmed by a toy model. The minimal output ellipticity was found at the wavelength of lowest loss near the center of the transmission band, whereas birefringence substantially increases toward the resonances. The analysis that qualitatively also applies to other kinds of hollow-core fibers showed that maximizing the amount of linearly polarized light at the fiber output demands both operating at the wavelength of lowest loss, as well as carefully choosing the relative orientation of input polarization. This should correspond to the situation in which the difference of the core extent along the two corresponding orthogonal polarization directions is minimal. Due to their practical relevance, we expect our findings to be very important in fields such as nonlinear photonics or metrology.

Origins of modal loss of antiresonant hollow-core optical fibers in the ultraviolet.

Recently, a novel antiresonant hollow core fiber was introduced having promising UV guiding properties. Accompanying simulations predicted ten times lower loss than observed experimentally. Increasing loss is observed in many antiresonant fibers with the origin being unknown. Here, two possible reasons for the enhanced loss are discussed: strand thickness variation and surface roughness scattering. Our analysis shows that the attenuation is sensitive to thickness variations of the strands surrounding the hollow-core which strongly increase loss at short wavelengths. The contribution of surface roughness stays below the dB/km level and can be neglected. Thus, preventing structural irregularities by improved fabrication approaches is essential for decreasing loss.

Low-loss single-mode guidance in large-core antiresonant hollow-core fibers.

We present an approach how to combine large-mode field diameters with effective single-mode guidance in a hollow-core antiresonant optical fiber. We demonstrate experimentally and in simulations that single-mode guidance is achieved in a simplified hollow-core fiber design with a core diameter of 30 µm by shifting the effective indices of the first cladding modes close to those of higher order core modes. Our fiber shows low loss propagation and effective single-mode operation from the near infrared to deep ultraviolet wavelengths down to 270 nm on a loss level of approximately 3 dB/m.

Double antiresonant hollow core fiber--guidance in the deep ultraviolet by modified tunneling leaky modes.

Guiding light inside the hollow cores of microstructured optical fibers is a major research field within fiber optics. However, most of current fibers reveal limited spectral operation ranges between the mid-visible and the infrared and rely on complicated microstructures. Here we report on a new type of hollow-core fiber, showing for the first time distinct transmission windows between the deep ultraviolet and the near infrared. The fiber, guiding in a single mode, operates by the central core mode being anti-resonant to adjacent modes, leading to a novel modified tunneling leaky mode. The fiber design is straightforward to implement and reveals beneficial features such as preselecting the lowest loss mode (Gaussian-like or donut-shaped mode). Fibers with such a unique combination of attributes allow accessing the extremely important deep-UV range with Gaussian-like mode quality and may pave the way for new discoveries in biophotonics, multispectral spectroscopy, photo-initiated chemistry or ultrashort pulse delivery.

From instable directional switching to controlled unidirectional operation in a nonlinear fiber ring laser.

We investigate a new phenomenon, where a reciprocal fiber ring laser switches from bidirectional to unidirectional operation above a certain pump power threshold. Significant simplifications regarding earlier experiments are presented, which for the first time allow the identification of individual nonlinear effects. We highlight the unique role of stimulated Raman scattering in triggering unidirectional operation, and that additional conditions apply. The threshold is reduced from 30 to 3.8 W, which eases potential applications.

Ultrafast Kapitza-Dirac effect.

Similar to the optical diffraction of light passing through a material grating, the Kapitza-Dirac effect occurs when an electron is diffracted by a standing light wave. In its original description, the effect is time independent. Here, we extended the Kapitza-Dirac effect to the time domain. By tracking the spatiotemporal evolution of a pulsed electron wave packet diffracted by a 60-femtosecond (where one femtosecond = 10-15 seconds) standing wave pulse in a pump-probe scheme, we observed time-dependent diffraction patterns. The fringe spacing in the observed pattern differs from that generated by the conventional Kapitza-Dirac effect. By exploiting this time-resolved diffraction scheme, we can access the time evolution of the phase properties of a free electron and potentially image ionic potentials and electronic decoherences.

Mode resolved bend loss in few-mode optical fibers.

We present a novel approach to directly measure the bend loss of individual modes in few-mode fibers based on the correlation filter technique. This technique benefits from a computer-generated hologram performing a modal decomposition, yielding the optical power of all propagating modes in the bent fiber. Results are compared with rigorous loss simulations and with common loss formulas for step-index fibers revealing high measurement fidelity. To the best of our knowledge, we demonstrate for the first time an experimental loss discrimination between index-degenerated modes.

Nanoscale all-normal dispersion optical fibers for coherent supercontinuum generation at ultraviolet wavelengths.

We report on the possibilities of nanoscale optical fibers with all-normal dispersion behavior for pulse-preserving and coherent supercontinuum generation at deep ultraviolet wavelengths. We discuss the influence of important parameters such as pump wavelength and fiber diameter, for both optical nanofibers and nanoscale suspended-core optical fibers. Simulations reveal that by appropriate combination of fiber geometry and input pulse parameters, intensive spectral components well below 300 nm are generated. In addition, the impact of preceding taper transitions used for input coupling purposes is discussed in detail.

Photoelectron energy peaks shift against the radiation pressure in strong-field ionization.

The photoelectric effect describes the ejection of an electron upon absorption of one or several photons. The kinetic energy of this electron is determined by the photon energy reduced by the binding energy of the electron and, if strong laser fields are involved, by the ponderomotive potential in addition. It has therefore been widely taken for granted that for atoms and molecules, the photoelectron energy does not depend on the electron's emission direction, but theoretical studies have questioned this since 1990. Here, we provide experimental evidence that the energies of photoelectrons emitted against the light propagation direction are shifted toward higher values, while those electrons that are emitted along the light propagation direction are shifted to lower values. We attribute the energy shift to a nondipole contribution to the ponderomotive potential that is due to the interaction of the moving electrons with the incident photons.

Pulse-preserving broadband visible supercontinuum generation in all-normal dispersion tapered suspended-core optical fibers.

Recently, coherent pulse-preserving and octave-spanning supercontinuum (SC) generation was theoretically predicted and experimentally shown in photonic crystal fibers (PCFs) with all-normal dispersion behavior. Since this behavior is due only to the all-normal dispersion profile and not to the photonic crystal cladding, other all-normal optical waveguides exhibit these properties as well. We extend this concept to suspended-core fibers and optical nanofibers and show experimental demonstrations of this way of SC generation. We show that optical suspended-core fibers and optical nanofibers of appropriate dimensions exhibit all-normal dispersion and address octave-spanning single pulse SC generation in the visible (VIS) and ultra violet (UV) wavelength range. In addition, we discuss the feasibility of fiber taper transitions for suitable input coupling schemes in sub-micron diameter fibers and show the importance of short adiabatic transition profiles for utilizing high-energy pulses to obtain maximum spectral broadening. They are essential for coherent broadband UV SC generation in optical nanofibers.

Design of all-normal dispersion microstructured optical fibers for pulse-preserving supercontinuum generation.

Recently, the generation of coherent, octave-spanning, and recompressible supercontinuum (SC) light has been demonstrated in optical fibers with all-normal group velocity dispersion (GVD) behavior by femtosecond pumping. In the normal dispersion regime, soliton dynamics are suppressed and the SC generation process is mainly due to self-phase modulation and optical wave breaking. This makes such white light sources suitable for time-resolved applications. The broadest spectra can be obtained when the pump wavelength equals the wavelength of maximum all-normal GVD. Therefore each available pump wavelength requires a specifically designed optical fiber with suitable GVD to unfold its full power. We investigate the possibilities to shift the all-normal maximum dispersion wavelength in microstructured optical fibers from the near infra red (NIR) to the ultra violet (UV). In general, a submicron guiding fiber core surrounded by a holey region is required to overcome the material dispersion of silica. Photonic crystal fibers (PCFs) with a hexagonal array of holes as well as suspended core fibers are simulated for this purpose over a wide field of parameters. The PCFs are varied concerning their air hole diameter and pitch and the suspended core fibers are varied concerning the number of supporting walls and the wall width. We show that these two fiber types complement each other well in their possible wavelength regions for all-normal GVD. While the PCFs are suitable for obtaining a maximum all-normal GVD in the NIR, suspended core fibers are well applicable in the visible wavelength range.

Coherent octave spanning near-infrared and visible supercontinuum generation in all-normal dispersion photonic crystal fibers.

We present the first detailed demonstrations of octave-spanning SC generation in all-normal dispersion photonic crystal fibers (ANDi PCF) in the visible and near-infrared spectral regions. The resulting spectral profiles are extremely flat without significant fine structure and with excellent stability and coherence properties. The key benefit of SC generation in ANDi PCF is the conservation of a single ultrashort pulse in the time domain with smooth and recompressible phase distribution. For the first time we confirm the exceptional temporal properties of the generated SC pulses experimentally and demonstrate their applicability in ultrafast transient absorption spectroscopy. The experimental results are in excellent agreement with numerical simulations, which are used to illustrate the SC generation dynamics by self-phase modulation and optical wave breaking. To our knowledge, we present the broadest spectra generated in the normal dispersion regime of an optical fiber.