Kilohertz droplet-on-demand serial femtosecond crystallography at the European XFEL station FXE.

X-ray Free Electron Lasers (XFELs) allow the collection of high-quality serial femtosecond crystallography data. The next generation of megahertz superconducting FELs promises to drastically reduce data collection times, enabling the capture of more structures with higher signal-to-noise ratios and facilitating more complex experiments. Currently, gas dynamic virtual nozzles (GDVNs) stand as the sole delivery method capable of best utilizing the repetition rate of megahertz sources for crystallography. However, their substantial sample consumption renders their use impractical for many protein targets in serial crystallography experiments. Here, we present a novel application of a droplet-on-demand injection method, which allowed operation at 47 kHz at the European XFEL (EuXFEL) by tailoring a multi-droplet injection scheme for each macro-pulse. We demonstrate a collection rate of 150 000 indexed patterns per hour. We show that the performance and effective data collection rate are comparable to GDVN, with a sample consumption reduction of two orders of magnitude. We present lysozyme crystallographic data using the Large Pixel Detector at the femtosecond x-ray experiment endstation. Significant improvement of the crystallographic statistics was made by correcting for a systematic drift of the photon energy in the EuXFEL macro-pulse train, which was characterized from indexing the individual frames in the pulse train. This is the highest resolution protein structure collected and reported at the EuXFEL at 1.38 Å resolution.

Probing of three-dimensional spin textures in multilayers by field dependent X-ray resonant magnetic scattering.

In multilayers of magnetic thin films with perpendicular anisotropy, domain walls can take on hybrid configurations in the vertical direction which minimize the domain wall energy, with Néel walls in the top or bottom layers and Bloch walls in some central layers. These types of textures are theoretically predicted, but their observation has remained challenging until recently, with only a few techniques capable of realizing a three dimensional characterization of their magnetization distribution. Here we perform a field dependent X-ray resonant magnetic scattering measurements on magnetic multilayers exploiting circular dichroism contrast to investigate such structures. Using a combination of micromagnetic and X-ray resonant magnetic scattering simulations along with our experimental results, we characterize the three-dimensional magnetic texture of domain walls, notably the thickness resolved characterization of the size and position of the Bloch part in hybrid walls. We also take a step in advancing the resonant scattering methodology by using measurements performed off the multilayer Bragg angle in order to calibrate the effective absorption of the X-rays, and permitting a quantitative evaluation of the out of plane (z) structure of our samples. Beyond hybrid domain walls, this approach can be used to characterize other periodic chiral structures such as skyrmions, antiskyrmions or even magnetic bobbers or hopfions, in both static and dynamic experiments.

Soft X-ray magnetic scattering studies of 3D magnetic morphology along buried interfaces in NiFe/CoPd/NiFe nanostructures.

With the continuing interest in new magnetic materials for sensor devices and data storage applications, the community needs reliable and sensitive tools for the characterization of such materials. Soft X-rays tuned to elemental absorption edges are a depth and element sensitive probe of magnetic structure at the nanoscale, and scattering measurements have the potential to provide 3D magnetic structural information of the material. In this work we develop a methodology in transmission geometry that allows one to probe the spatial distribution of the magnetization along the different layers of magnetic heterostructures. We study the in-plane/out-of-plane transition of magnetic domains in multilayer thin film systems consisting of two layers of NiFe top and bottom, and a 50 repeat Co/Pd multilayer in the centre. The experimental data are analysed by simulating scattering data starting from micromagnetic simulations, and we find that the out of plane domains of the Co/Pd multilayer intrude into the NiFe layers to a greater extent than would be expected from micromagnetic simulations performed using the standard magnetically isotropic input parameters for the NiFe layers.

Micro X-ray Fluorescence Study of Late Pre-Hispanic Ceramics from the Western Slopes of the South Central Andes Region in the Arica y Parinacota Region, Chile: A New Methodological Approach.

Archeological ceramic paste material typically consists of a mix of a clay matrix and various millimeter and sub-millimeter sized mineral inclusions. Micro X-ray fluorescence (XRF) is a standard compositional classification tool and in this work we propose and demonstrate an improved fluorescence map processing protocol where the mineral inclusions are automatically separated from the clay matrix to allow independent statistical analysis of the two parts. Application of this protocol allowed us to enhance the discrimination between different ceramic shards compared with the standard procedure of working with only the spatially averaged elemental concentrations. Using the new protocol, we performed an initial compositional classification of a set of 83 ceramic shards from the western slopes of the south central Andean region in the Arica y Parinacota region (Chile). Comparing the classifications obtained using the new versus the old (average concentrations only) protocols, we found that some samples were erroneously classified with the old protocol. From an archaeological perspective, a broad and heterogeneous regional sample set was used in this experimental study due to the fact that this was the first such analysis to be performed on ceramics from this region. This allowed a general overview to be obtained, however further work on more specific sample sets will be necessary to extract concrete archaeological conclusions.

Method for single-shot coherent diffractive imaging of magnetic domains.

In preparation for real space studies of magnetic domains in a pump-probe setup at free-electron laser sources, it is necessary to develop an imaging method compatible with the linearly polarized radiation available at these sources. We present results from a prototype experiment performed at the synchrotron source BESSY II, using a modification of existing phase retrieval techniques. Our results show that it is possible to image magnetic domains in real space using linear polarized light, and we introduce the concept of a reliability map of our reconstructions using Gabor transforms.

Experimental geometry for simultaneous beam characterization and sample imaging allowing for pink beam Fourier transform holography or coherent diffractive imaging.

One consequence of the self-amplified stimulated emission process used to generate x rays in free electron lasers (FELs) is the intrinsic shot-to-shot variance in the wavelength and temporal coherence. In order to optimize the results from diffractive imaging experiments at FEL sources, it will be advantageous to acquire a means of collecting coherence and spectral information simultaneously with the diffraction pattern from the sample we wish to study. We present a holographic mask geometry, including a grating structure, which can be used to extract both temporal and spatial coherence information alongside the sample scatter from each individual FEL shot and also allows for the real space reconstruction of the sample using either Fourier transform holography or iterative phase retrieval.

Recovering magnetization distributions from their noisy diffraction data.

We study, using simulated experiments inspired by thin-film magnetic domain patterns, the feasibility of phase retrieval in x-ray diffractive imaging in the presence of intrinsic charge scattering given only photon-shot-noise limited diffraction data. We detail a reconstruction algorithm to recover the sample's magnetization distribution under such conditions and compare its performance with that of Fourier transform holography. Concerning the design of future experiments, we also chart out the reconstruction limits of diffractive imaging when photon-shot-noise and the intensity of charge scattering noise are independently varied. This work is directly relevant to the time-resolved imaging of magnetic dynamics using coherent and ultrafast radiation from x-ray free-electron lasers and also to broader classes of diffractive imaging experiments which suffer noisy data, missing data, or both.

Extracting coherent modes from partially coherent wavefields.

A method for numerically recovering the coherent modes and their occupancies from a known mutual optical intensity function is described. As an example, the technique is applied to previously published experimental data from an x-ray undulator source. The data are found to be described by three coherent modes, and the functional forms and relative occupancies of these modes are recovered.