Simultaneous two-color snapshot view on ultrafast charge and spin dynamics in a Fe-Cu-Ni tri-layer.

Ultrafast phenomena on a femtosecond timescale are commonly examined by pump-probe experiments. This implies multiple measurements, where the sample under investigation is pumped with a short light pulse and then probed with a second pulse at various time delays to follow its dynamics. Recently, the principle of streaking extreme ultraviolet (XUV) pulses in the temporal domain has enabled recording the dynamics of a system within a single pulse. However, separate pump-probe experiments at different absorption edges still lack a unified timing, when comparing the dynamics in complex systems. Here, we report on an experiment using a dedicated optical element and the two-color emission of the FERMI XUV free-electron laser to follow the charge and spin dynamics in composite materials at two distinct absorption edges, simultaneously. The sample, consisting of ferromagnetic Fe and Ni layers, separated by a Cu layer, is pumped by an infrared laser and probed by a two-color XUV pulse with photon energies tuned to the M-shell resonances of these two transition metals. The experimental geometry intrinsically avoids any timing uncertainty between the two elements and unambiguously reveals an approximately 100 fs delay of the magnetic response with respect to the electronic excitation for both Fe and Ni. This delay shows that the electronic and spin degrees of freedom are decoupled during the demagnetization process. We furthermore observe that the electronic dynamics of Ni and Fe show pronounced differences when probed at their resonance, while the demagnetization dynamics are similar. These observations underline the importance of simultaneous investigation of the temporal response of both charge and spin in multi-component materials. In a more general scenario, the experimental approach can be extended to continuous energy ranges, promising the development of jitter-free transient absorption spectroscopy in the XUV and soft X-ray regimes.

LamNI - an instrument for X-ray scanning microscopy in laminography geometry.

Across all branches of science, medicine and engineering, high-resolution microscopy is required to understand functionality. Although optical methods have been developed to `defeat' the diffraction limit and produce 3D images, and electrons have proven ever more useful in creating pictures of small objects or thin sections, so far there is no substitute for X-ray microscopy in providing multiscale 3D images of objects with a single instrument and minimal labeling and preparation. A powerful technique proven to continuously access length scales from 10 nm to 10 µm is ptychographic X-ray computed tomography, which, on account of the orthogonality of the tomographic rotation axis to the illuminating beam, still has the limitation of necessitating pillar-shaped samples of small (ca 10 µm) diameter. Large-area planar samples are common in science and engineering, and it is therefore highly desirable to create an X-ray microscope that can examine such samples without the extraction of pillars. Computed laminography, where the axis of rotation is not perpendicular to the illumination direction, solves this problem. This entailed the development of a new instrument, LamNI, dedicated to high-resolution 3D scanning X-ray microscopy via hard X-ray ptychographic laminography. Scanning precision is achieved by a dedicated interferometry scheme and the instrument covers a scan range of 12 mm × 12 mm with a position stability of 2 nm and positioning errors below 5 nm. A new feature of LamNI is a pair of counter-rotating stages carrying the sample and interferometric mirrors, respectively.

Towards optimized illumination for high-resolution ptychography.

We present a systematic study, where effects of the illumination probe design on ptychography reconstruction quality are evaluated under well-controlled conditions. The illumination probe was created using Fresnel zone-plate (FZP) optics with locally displaced zones to provide a fine control over perturbations of the illumination wavefront. We show that optimally designed wavefront modulations not only reduce bias and variance in the reconstruction of the lowest spatial frequencies but also lead to improved imaging resolution and reduction of artefacts compared to a conventional FZP. Both these factors are important for quantitative accuracy and resolution of ptychographic tomography. Our work furthers the understanding of the important characteristics of an optimal illumination for high-resolution X-ray ptychography and how to design optimal FZP wavefront modulations for different applications of ptychographic imaging. These findings are applicable and relevant for ptychography using optical, EUV, and X-ray photons as well as electrons.

Fast positioning for X-ray scanning microscopy by a combined motion of sample and beam-defining optics.

Scanning X-ray microscopy such as X-ray ptychography requires accurate and fast positioning of samples in the X-ray beam. Sample stages often have a high mobile mass as they may carry additional mechanics or mirrors for position measurements. The high mobile mass of a piezo stage can introduce vibrations in the setup that will lead to imaging quality deterioration. Sample stages also require a large travel range which results in a slow positioning step response and thus high positioning overhead. Moving lightweight X-ray optics, such as focusing Fresnel zone plates, instead of the sample can improve the situation but it may lead to undesired variations in the illumination probe which may result in reconstruction artifacts. This paper presents a combined approach in which a slow sample stage mechanism covers the long distance range for a large field of view, and a light-weight optics scanner with a small travel range creates a superimposed motion to achieve a fast step response. The step response in the ptychographic tomography instrument used was thereby improved by an order of magnitude, allowing for efficient measurement without loss of imaging quality.

High-intensity x-ray microbeam for macromolecular crystallography using silicon kinoform diffractive lenses.

Macromolecular crystallography often requires focused high-intensity x-ray beams for solving challenging protein structures from micrometer-sized crystals using current synchrotron radiation sources. The design of optical focusing schemes for hard x-rays showing high efficiency and flexibility in beam size is therefore continuously pursued. Here, we present an innovative solution based on a two-stage demagnification of the undulator source for photon energies from 6 keV to 19 keV, commissioned at the X10SA beamline of the Swiss Light Source, where a secondary source is imaged by two crossed silicon kinoform x-ray diffractive lenses with 75 nm outermost zone width. A source-size limited spot with a size of 4.8 µm×1.7 µm(h×v,FWHM) and flux of 7.5×1010 photons/s at 12.4 keV is demonstrated at the sample position.

High-acceptance versatile microfocus module based on elliptical Fresnel zone plates for small-angle X-ray scattering.

High-efficiency microfocusing of multi-keV X-rays at synchrotron sources is highly profitable for spatially resolved structural analysis of many kinds. Because radiation from synchrotron sources is typically elongated along the horizontal dimension, generating a microbeam that is isotropic in size requires a carefully designed optics system. Here we report on using a combination of a horizontally tunable slit downstream of the undulator source with elliptical diffractive Fresnel zone plates. We demonstrate the arrangement in context of small-angle X-ray scattering experiments, obtaining a microbeam of 2.2 µm × 1.8 µm (X × Y) with a flux of 1.2 × 1010 photons/s at an energy of 11.2 keV at the sample position.

Implementation of quantum and classical discrete fractional Fourier transforms.

Fourier transforms, integer and fractional, are ubiquitous mathematical tools in basic and applied science. Certainly, since the ordinary Fourier transform is merely a particular case of a continuous set of fractional Fourier domains, every property and application of the ordinary Fourier transform becomes a special case of the fractional Fourier transform. Despite the great practical importance of the discrete Fourier transform, implementation of fractional orders of the corresponding discrete operation has been elusive. Here we report classical and quantum optical realizations of the discrete fractional Fourier transform. In the context of classical optics, we implement discrete fractional Fourier transforms of exemplary wave functions and experimentally demonstrate the shift theorem. Moreover, we apply this approach in the quantum realm to Fourier transform separable and path-entangled biphoton wave functions. The proposed approach is versatile and could find applications in various fields where Fourier transforms are essential tools.

Experimental observation of N00N state Bloch oscillations.

Bloch oscillations of quantum particles manifest themselves as periodic spreading and relocalization of the associated wave functions when traversing lattice potentials subject to external gradient forces. Albeit this phenomenon is deeply rooted into the very foundations of quantum mechanics, all experimental observations so far have only contemplated dynamics of one and two particles initially prepared in separable local states. Evidently, a more general description of genuinely quantum Bloch oscillations will be achieved on excitation of a Bloch oscillator by nonlocal states. Here we report the observation of Bloch oscillations of two-particle N00N states, and discuss the nonlocality on the ground of Bell-like inequalities. The time evolution of two-photon N00N states in Bloch oscillators, whether symmetric, antisymmetric or partially symmetric, reveals transitions from particle antibunching to bunching. Consequently, the initial states can be tailored to produce spatial correlations akin to those of bosons, fermions and anyons, presenting potential applications in photonic quantum simulation.