Conference Agenda

Fourth-generation synchrotron X-ray sources bring increasing levels of flux and coherence, allowing unprecedented levels of resolution for a wide range of techniques, but with increasing risk of radiation damage. The high flux achievable at synchrotrons has been well known to cause damage in biological samples at around 5-20 keV, however, with increasing flux we have found that radiation effects become significant even for metal samples and high-energy X-rays through beam heating.

Beam heating effects were investigated at the ID11 beamline at the newly upgraded European Synchrotron Radiation Facility-Extremely Brilliant Source, using thermal lattice expansion to perform in-situ measurements. Results showed significant increases in temperature for metal and ceria samples in a focussed 43.44 keV beam, as displayed in Fig. 1. These temperature increases may affect sample properties and drive significant chemical or physical changes, such as the rapid recrystallisation of copper wire shown here.

Aluminium and Copper wire samples were investigated and compared to a lumped thermodynamic model. By designing samples to maximise effects and simplify the thermodynamics of the system, we facilitate quantitative comparison to the modelled beam heating, helping to understand the severity of the problem. With these results we show that radiation beam heating is a potential issue for all samples, not only soft matter, and provide information needed to consider, predict, and mitigate its effects.

With the onset of next generation synchrotron light sources and X-ray free electron lasers, accompanied by developments of future photon detectors, delivering mega-pixel diffraction images at frame rates over 10 kHz, production of data from crystallography experiments is rapidly increasing. Crystallographers were utilizing various types of computing hardware from the early beginning. Algorithms and computing devices were constantly developing. Nowadays even quantum computers are available in commercial clouds. A potential of Field-Programmable Gate Arrays (FPGAs) – a more classical computing accelerators, is explored and demonstrated in this work on a task of Azimuthal Integration (AZINT) of area-detector data from powder diffraction and small angle scattering. Beside these two most known application cases, where among other data volumes are reduced by a factor of 1000, the underlaying procedure i.e. bin-counting has applications in data analysis tasks as background estimation in conventional single crystal diffraction images or data reduction from diffraction anomalous fine structure. The new potential of FPGAs for big data science and complex data analysis originates from recent progress in tools allowing scientific software developers to easily program FPGAs, prototype and implement algorithms on them with complexity fitting the scientific requirements. It is demonstrated that AZINT can process 600 Gb/s of uncompressed data stream, i.e. about 20–40 Gpixels/s, on a single commercial FPGA available at photon and neutron facilities or compute clouds, however energy and cost-effective commodity hardware FPGAs can be used as well. FPGAs are usually more energy-efficient in comparison to widely known graphical processing units (GPUs) and they are very flexible so they can better fit a specific problem and outperform GPUs in many relevant applications, in particular AZINT here. Beside high throughput required for big data analysis FPGAs allow data reduction and filtering with well-defined and low latencies. This enables experiments with X-rays as a real-time probe. Development of crystallographic code for big data handling on FPGAs may have additional synergies. FPGAs can be radiation tolerant and operate under some extreme conditions. It makes them ideal components for extra-terrestrial crystallography (e.g. Mars rovers). AZINT was developed at MAX IV synchrotron Laboratory however similar activities are present on other photon sources. It is worth to mention at least data acquisition and spot-finding project [1] for macromolecular crystallography at SLS/PSI.

[1] Leonarski, F., Mozzanica, A., Brückner, M., Lopez-Cuenca, C., Redford, S., Sala, L., Babic, A., Billich, H., Bunk, O., Schmitt, B., Wang, M. (2020). Structural Dynamics 7, 014305. https://doi.org/10.1063/1.5143480

Simultaneous recording of diffraction patterns in a large solid angle with the subsequent conversion of a two-dimensional histogram into a one-dimensional intensity – diffraction angle dependence [I (2θ)] is obviously a highly efficient data collection method for polycrystalline samples, the diffraction pattern of which is axially symmetric. This approach provides a high measurement rate with the required statistical accuracy. Shooting time is smaller by orders of magnitude compared to a point or linear detector. The negative effect of graininess and preferential orientation (texture) on data quality is reduced. However, due to the limited size of two-dimensional detectors, the resulting angular range is very limited and insufficient to obtain accurate structural information about the studied objects. In this regard, the principle of a scanning two-dimensional detector was used at the X-ray structural analysis beamline (XSA) mounted on a beam from a bending magnet of Kurchatov Synchrotron Radiation Source. The optical scheme is standard and includes a monochromator with a sagittal bend of the second crystal to focus the beam in the horizontal plane to obtain maximum intensity values [1].

The goniometer provides rotation of the test sample (placed in a special cryoloop or thin-walled capillary) around the horizontal axis φ, to ensure averaging of diffraction patterns over the orientations of the sample, as well as rotation of the detector around the 2θ axis, which allows high quality data to be obtained up to large values ​​of sinθ / λ. The use of such a scheme made it possible to obtain the following parameters of the diffraction experiment:

• an angular range of up to 140⁰ in 2θ (q = 14.8 Å^-1)
• instrumental contribution to the peak broadening from 0.039⁰
• angular accuracy Δ2θ = 0.001 °,
• the accuracy of determining the intensities of the Bragg peaks of the standard – 0.5%,
• the range of recorded intensities of the Bragg peaks Imax / Imin = 10⁵.

[1] Svetogorov R.D., Dorovatovskii P.V., Lazarenko V.A. (2020) Cryst. Res. Tech. in press

The Advanced Photon Source (APS) at Argonne National Laboratory has played a major role in the materials and applied science research for 25 years. Now the source will be upgraded starting in April 2023 [1,2]. In 2024, users can expect an ultra-bright source operated at 6 GeV with high fraction of coherence even at high-energy x-ray. There will be 9 new feature beamlines built to take full advantage of the new source parameter, and many beamlines will become enhanced including insertion devices, optics, and instrumentation.

11-ID-D operated by the Structural Science group at the APS is one of the enhanced beamlines, which will enable a combination of total scattering with small angle scattering and focusing into the submicrometer range. Here, we can close the gap between the resolution in reciprocal and real space to provide a complete picture of the structure of materials. Multimodal setups and photon energies between 26 keV and 120 keV with highest flux will enable complex in situ and operando experiments. An emphasis will be on the understanding and discovery of new materials covering in situ synthesis and manufacturing to studies during functionality.

[1] https://www.aps.anl.gov/APS-Upgrade

[2] Advanced Photon Source Upgrade Project Preliminary Design Report https://doi.org/10.2172/1423830

Keywords: synchrotron radiation; powder diffraction; total scattering; nanomaterials; materials science

Acknowledgement: This research used resources of the Advanced Photon Source, a U.S. Department of Energy (DOE) Office of Science User Facility, operated for the DOE Office of Science by Argonne National Laboratory under Contract No. DE-AC02-06CH11357.

The arrival of the 4^th Generation Synchrotron Rings (4GSR) facilitates a crucial step forward in the application range of modern X-ray methods. The 4GSR sources pave a way for time resolved experiments at nanometer and nanosecond resolution level and beyond. Their development therefore allows for moving the established scattering, diffraction and spectroscopy methods to the nanoscale, to combine them with microscopy at mesoscopic levels and to investigate dynamics at nanosecond time scales. The Russian national flagship Ultimate Source for Synchrotron Radiation (USSR) facility will be one of the world leading synchrotrons once it starts operation.

A major part of the existing 4GSR beamlines is dedicated to nanobeam experiments. The intended X-ray research methods must be capable of obtaining the information of the real structure at nanometer resolution levels. The required spatial resolution on the objects can vary from several interatomic spaces in modern microelectronic devices, lithium-based batteries and catalytic materials and up to tens of micrometers e. g. in research on mechanical fails or stress propagation. Moreover, the key interest concentrates on the evolution of the objects, under external influences or in the cause of device operation. Because of this great interest in nanobeam experiments, the conceptual design of nano-diffraction beamlines is of primary interest in the preparation phase of USSR.

Here, we present an analysis of the scientific cases and developments of conceptual and technical solutions for the design of a scattering/diffraction beamline. This study includes a broad overview of recent scientific cases investigated at nowadays beamlines with similar focus. Additionally, we present an extensive comparison of Nanoprobe Beamlines at 4GSR that are already operating or under construction. From those key data, we derive a model beamline for nanoprobe experiments at USSR. This generic beamline consists of (1) a double-crystal monochromator Si(111) with a bandwidth of 10^-4, covering an energy range of 5 keV to 40 keV, (2) a 4m long tunable undulator (see Fig. 1), (3) two different combinations of focusing elements and (4) a 4+2 circle diffractometer. The beam properties of these concepts were modelled with the x-ray tracing software xrt at different positions of the beamline. The minimal beam size at the sample position is 220nm x 70nm (FWHM), see Fig. 2.

As the first macromolecular crystallography (MX) beamline at a fourth-generation synchrotron source, BioMAX [1] is also the first MX beamline at the MAX IV Laboratory. The primary usage case has targeted high sample throughput and robustness, using the performance of the MAX IV source to achieve a 20 x 5 μm² beam focus with few beam shaping elements. Operation of the KB-mirror pair used for focusing, is automated to also deliver a defocused beam size of 50 x 50 or 100 x 100 μm². Using a double crystal Si(111) monochromator, an energy range of 5 to 25 keV is user accessible and a photon flux of 5 x 10¹² photon/s is routinely achieved at a ring current of 250 mA and a photon energy of 13 keV.

The beamline endstation has been based around well-established components such as the MD3 diffractometer from Arinax, a Dectris Eiger 16M photon counting detector and an IRELEC ISARA sample changer. The beamline is accommodating to a wide range of experiment types, including: cryogenic data collection, humidity-controlled room temperature data collection, optimised SAD/MAD capability, serial crystallography by fixed-target supports or injectors [2], helical data collection, rapid-feedback mesh scans and with a suite of auto-processing pipelines.

Also associated with the beamline is the FragMAX fragment screening program at MAX IV [3]. Beamline control is provided through the web-technology based MXCuBE3 [4] and with the ISPyB database [5] for LIMS functionality via the EXI user interface.

[1] Ursby, T., Åhnberg, K., Appio, R., Aurelius, O., Barczyk, A., Bartalesi, A., Bjelčić, M., Bolmsten, F., Cerenius, Y., Doak, R. B., Eguiraun, M., Eriksson, T., Friel, R. J., Gorgisyan, I., Gross, A., Haghighat, V., Hennies, F., Jagudin, E., Norsk Jensen, B., Jeppsson, T., Kloos, M., Li-don-Simon, J., de Lima, G. M. A., Lizatovic, R., Lundin, M., Milan-Otero, A., Milas, M., Nan, J., Nardella, A., Rosborg, A., Shilova, A., Shoeman, R. L., Siewert, F., Sondhauss, P., Talibov, V., Tarawneh, H., Thånell, J., Thunnissen, M., Unge, J., Ward, C., Gonzalez, A. & Mueller, U. (2020). J. Synchrotron Radiat. 27, 1415. DOI:10.1107/s1600577520008723

[2] Shilova, A., Lebrette, H., Aurelius, O., Nan, J., Welin, M., Kovacic, R., Ghosh, S., Safari, C., Friel, R. J., Milas, M., Matej, Z., Högbom, M., Brändén, G., Kloos, M., Shoeman, R. L., Doak, B., Ursby, T., Håkansson, M., Logan, D. T. & Mueller, U. (2020). J. Synchrotron Radiat. 27, 1095. DOI: 10.1107/S1600577520008735

[3] Lima, G.M.A., Talibov, V.O., Jagudin, E., Sele, C., Nyblom, M., Knecht, W., Logan, D.T., Sjögren, T. & Mueller, U. (2020). Acta Crystallogr. D. 76, 771. DOI: 10.1107/S205979832000889X

[4] Mueller, U., Thunnissen, M., Nan, J., Eguiraun, M., Bolmsten, F., Milàn-Otero, A., Guijarro, M., Oscarsson, M., de Sanctis, Daniele. & Leonard, G. A. (2017). Synchrotron Radiat. News 30, 22. DOI: 10.1080/08940886.2017.1267564

[5] Delagenière, S., Brenchereau, P., Launer, L., Ashton, A. W., Leal, R., Veyrier, S., Gabadinho, J., Gordon, E. J., Jones, S. D., Levik, K. E., McSweeney, S. M., Monaco, S., Nanao, M., Spruce, D., Svensson, O., Walsh, M. A. & Leonard, G. A. (2011). Bioinformatics 27 (22), 3186. DOI: 10.1093/bioinformatics/btr535

Since 2016 the Chemical Crystallography beamline P24 at the synchrotron Petra III located at DESY Hamburg is offering user operation. The two experimental hutches EH1 and EH2 are equipped with a large kappa-geometry diffractometer and a four circle eulerian-craddle diffractometer respectively. In recent years serveral improvements have been added in order to facilitate small molecule chemical crystallography in particular the determination of routine crystal structures from extremely small single crystals unsuitable for home laboratory X-ray diffractometers.

At present the available energies (wavelengths) encompasses an small window at 8 keV (1.54 Å) and the range from 17 to 30 keV (0.73 to 0.41 Å). Higher energies up to 40 keV are technically possible. A Pilatus 3R 1M cadmiumtelluride hybridpixel detector in addition to a Mar 165 CCD are available in either experimental hutch, together with low temperature gas flow coolers, down to helium temperatures. A set of recently installed compound refractive lenses (CRLs) allows to focus the beam to below 100 μm. Presently in EH1 a sample changing collaborative robot is being tested, together with a new fixed Chi sample stage, which allows for omega scans exceeding 180° in combination with predefined Phi-settings. An automated goniometer head allows to centre the crystal remotely.

A low temperature sample storage accessible for the robot is planned for the near future. This will complete the setup for possible remote operation of the beamline by EH1 users including a mail-in service for air, humidity and temperature sensitive samples.

In 2024, the upgrade of the Advanced Photon Source at Argonne National Laboratory to an MBA reverse bent lattice will be completed. APS-U will offer extremely brilliant and highly coherent beam through the new low emittance source [1] to the user community. This will enable a variety of exciting new possibilities for dichroic scattering and spectroscopy experiments by pushing towards extreme pressures and high spatial resolution. Polar, the beamline for polarization modulation spectroscopy at sector 4 of the APS will make use of these new possibilities in terms of small focus sizes, coherence and polarization.

Fast polarization flipping between left and right circular as well as between horizontal and vertical linear polarization will be possible with the new Superconducting Arbitrarily Polarizing Emitter (SCAPE) undulators which are currently being designed for the Polar beamline. Two in-line SCAPE undulators will produce horizontal and vertical linear polarization as well as left and right circular polarization in the energy range from 2.7 to 27 keV, thanks to the implementation of small diameter round ID vacuum chambers enabled by on-axis injection at APS-U. Two experimental setups will make use of this new source and will allow diffraction (XRD, REXS, XRMR) as well as absorption spectroscopy (XMCD, XMLD) experiments covering all relevant absorption edges.

The beamline will make accessible especially the energy range above 14 keV for magnetic spectroscopy experiments, normally not reachable at conventional hard-x-ray beamlines using phase plates for polarization manipulation and will enable investigation of magnetic properties of materials at the 5f L- and 4d K-edges using spectroscopic methods. Small focused and coherent beams down to 100 nm will allow reaching new areas in terms of resolution, by employing direct imaging or ptychographic methods, at low temperature, high magnetic fields and high pressures. Beamline optics are designed to reduce vibrations to guarantee small focus sizes.

A low vibration, large bore superconducting magnet with 9 T longitudinal and 1 T transversal fields will allow XMCD and XMLD measurements at extreme pressures using the small beam focused by KB optics. A horizontal diffractometer with an optional 2 T superconducting magnet will allow dichroic diffraction and spectroscopy experiments in moderate fields and at high pressures. An interchangeable high-precision sample stage will allow for 3D dichroic imaging experiments using highly focused beam.

[1] https://www.aps.anl.gov/Beamline-Selection/Technical-Information/Storage-Ring-Parameters