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Instruments / Technical Area	Publication Details	Published
	Development of crystal optics for X-ray multi-projection imaging for synchrotron and XFEL sources Valerio Bellucci , Sarlota Birnsteinova , Tokushi Sato , Romain Letrun , Jayanath C. P. Koliyadu , Chan Kim , Gabriele Giovanetti , Carsten Deiter , Liubov Samoylova , Ilia Petrov , Luis Lopez Morillo , Rita Graceffa , Luigi Adriano , Helge Huelsen , Heiko Kollmann , Thu Nhi Tran Calliste , Dusan Korytar , Zdenko Zaprazny , Andrea Mazzolari , Marco Romagnoni , Eleni Myrto Asimakopoulou , Zisheng Yao , Yuhe Zhang , Jozef Ulicny , Alke Meents , Henry N. Chapman , Richard Bean , Adrian Mancuso , Pablo Villanueva-Perez , Patrik Vagovic Journal Of Synchrotron Radiation 31 DOI: 10.1107/S1600577524008488 Open Access Show Abstract ▼ Abstract: X-ray multi-projection imaging (XMPI) is an emerging experimental technique for the acquisition of rotation-free, time-resolved, volumetric information on stochastic processes. The technique is developed for high-brilliance light-source facilities, aiming to address known limitations of state-of-the-art imaging methods in the acquisition of 4D sample information, linked to their need for sample rotation. XMPI relies on a beam-splitting scheme, that illuminates a sample from multiple, angularly spaced viewpoints, and employs fast, indirect, X-ray imaging detectors for the collection of the data. This approach enables studies of previously inaccessible phenomena of industrial and societal relevance such as fractures in solids, propagation of shock waves, laser-based 3D printing, or even fast processes in the biological domain. In this work, we discuss in detail the beam-splitting scheme of XMPI. More specifically, we explore the relevant properties of X-ray splitter optics for their use in XMPI schemes, both at synchrotron insertion devices and XFEL facilities. Furthermore, we describe two distinct XMPI schemes, designed to faciliate large samples and complex sample environments. Finally, we present experimental proof of the feasibility of MHz-rate XMPI at the European XFEL. This detailed overview aims to state the challenges and the potential of XMPI and act as a stepping stone for future development of the technique.	Nov 2024
	Development of MHz X-ray phase contrast imaging at the European XFEL Jayanath C. P. Koliyadu , Daniel Moško , Eleni Myrto Asimakopoulou , Valerio Bellucci , Šarlota Birnšteinová , Richard Bean , Romain Letrun , Chan Kim , Henry Kirkwood , Gabriele Giovanetti , Nerea Jardon , Janusz Szuba , Trey Guest , Andreas Koch , Jan Grünert , Peter Szeles , Pablo Villanueva-Perez , Fabian Reuter , Claus-Dieter Ohl , Mike Andreas Noack , Francisco Garcia-Moreno , Zuzana Kuglerová-Valdová , Libor Juha , Martin Nikl , Wataru Yashiro , Hitoshi Soyama , Daniel Eakins , Alexander M. Korsunsky , Jozef Ulicny , Alke Meents , Henry N. Chapman , Adrian P. Mancuso , Tokushi Sato , Patrik Vagovic Journal Of Synchrotron Radiation 32 DOI: 10.1107/S160057752400986X Show Abstract ▼ Abstract: We report on recent developments that enable megahertz hard X-ray phase contrast imaging (MHz XPCI) experiments at the Single Particles, Clusters, and Biomolecules and Serial Femtosecond Crystallography (SPB/SFX) instrument of the European XFEL facility (EuXFEL). We describe the technical implementation of the key components, including an MHz fast camera and a modular indirect X-ray microscope system based on fast scintillators coupled through a high-resolution optical microscope, which enable full-field X-ray microscopy with phase contrast of fast and irreversible phenomena. The image quality for MHz XPCI data showed significant improvement compared with a pilot demonstration of the technique using parallel beam illumination, which also allows access to up to 24 keV photon energies at the SPB/SFX instrument of the EuXFEL. With these developments, MHz XPCI was implemented as a new method offered for a broad user community (academic and industrial) and is accessible via standard user proposals. Furthermore, intra-train pulse diagnostics with a high few-micrometre spatial resolution and recording up to 128 images of consecutive pulses in a train at up to 1.1 MHz repetition rate is available upstream of the instrument. Together with the diagnostic camera upstream of the instrument and the MHz XPCI setup at the SPB/SFX instrument, simultaneous two-plane measurements for future beam studies and feedback for machine parameter tuning are now possible.	Nov 2024
B21-High Throughput SAXS	Microsecond time-resolved X-ray scattering by utilizing MHz repetition rate at second-generation XFELs Patrick E. Konold , Leonardo Monrroy , Alfredo Bellisario , Diogo Filipe , Patrick Adams , Roberto Alvarez , Richard Bean , Johan Bielecki , Szabolcs Bódizs , Gabriel Ducrocq , Helmut Grubmueller , Richard A. Kirian , Marco Kloos , Jayanath C. P. Koliyadu , Faisal H. M. Koua , Taru Larkiala , Romain Letrun , Fredrik Lindsten , Michael Maihöfer , Andrew Martin , Petra Mészáros , Jennifer Mutisya , Amke Nimmrich , Kenta Okamoto , Adam Round , Tokushi Sato , Joana Valerio , Daniel Westphal , August Wollter , Tej Varma Yenupuri , Tong You , Filipe Maia , Sebastian Westenhoff Nature Methods 17 DOI: 10.1038/s41592-024-02344-0 Open Access Show Abstract ▼ Abstract: Detecting microsecond structural perturbations in biomolecules has wide relevance in biology, chemistry and medicine. Here we show how MHz repetition rates at X-ray free-electron lasers can be used to produce microsecond time-series of protein scattering with exceptionally low noise levels of 0.001%. We demonstrate the approach by examining Jɑ helix unfolding of a light-oxygen-voltage photosensory domain. This time-resolved acquisition strategy is easy to implement and widely applicable for direct observation of structural dynamics of many biochemical processes.	Jul 2024
	Resolving nonequilibrium shape variations among millions of gold nanoparticles Zhou Shen , Paul Lourdu Xavier , Richard Bean , Johan Bielecki , Martin Bergemann , Benedikt Daurer , Tomas Ekeberg , Armando D. Estillore , Hans Fangohr , Klaus Giewekemeyer , Mikhail Karnevskiy , Richard A. Kirian , Henry Kirkwood , Yoonhee Kim , Jayanath C. P. Koliyadu , Holger Lange , Romain Letrun , Jannik Lübke , Abhishek Mall , Thomas Michelat , Andrew J. Morgan , Nils Roth , Amit K. Samanta , Tokushi Sato , Marcin Sikorski , Florian Schulz , Patrik Vagovic , Tamme Wollweber , Lena Worbs , Filipe Maia , Daniel A. Horke , Jochen Küpper , Adrian P. Mancuso , Henry Chapman , Kartik Ayyer , N. Duane Loh Acs Nano DOI: 10.1021/acsnano.4c00378 Open Access Show Abstract ▼ Abstract: Nanoparticles, exhibiting functionally relevant structural heterogeneity, are at the forefront of cutting-edge research. Now, high-throughput single-particle imaging (SPI) with X-ray free-electron lasers (XFELs) creates opportunities for recovering the shape distributions of millions of particles that exhibit functionally relevant structural heterogeneity. To realize this potential, three challenges have to be overcome: (1) simultaneous parametrization of structural variability in real and reciprocal spaces; (2) efficiently inferring the latent parameters of each SPI measurement; (3) scaling up comparisons between 105 structural models and 106 XFEL-SPI measurements. Here, we describe how we overcame these three challenges to resolve the nonequilibrium shape distributions within millions of gold nanoparticles imaged at the European XFEL. These shape distributions allowed us to quantify the degree of asymmetry in these particles, discover a relatively stable “shape envelope” among nanoparticles, discern finite-size effects related to shape-controlling surfactants, and extrapolate nanoparticles’ shapes to their idealized thermodynamic limit. Ultimately, these demonstrations show that XFEL SPI can help transform nanoparticle shape characterization from anecdotally interesting to statistically meaningful.	May 2024
	Revealing the origins of vortex cavitation in a Venturi tube by high speed X-ray imaging Hitoshi Soyama , Xiaoyu Liang , Wataru Yashiro , Kentaro Kajiwara , Eleni Myrto Asimakopoulou , Valerio Bellucci , Sarlota Birnsteinova , Gabriele Giovanetti , Chan Kim , Henry J. Kirkwood , Jayanath C. P. Koliyadu , Romain Letrun , Yuhe Zhang , Jozef Ulicny , Richard Bean , Adrian P. Mancuso , Pablo Villanueva-Perez , Tokushi Sato , Patrik Vagovic , Daniel Eakins , Alexander M. Korsunsky Ultrasonics Sonochemistry 101 DOI: 10.1016/j.ultsonch.2023.106715 Open Access Show Abstract ▼ Abstract: Hydrodynamic cavitation is useful in many processing applications, for example, in chemical reactors, water treatment and biochemical engineering. An important type of hydrodynamic cavitation that occurs in a Venturi tube is vortex cavitation known to cause luminescence whose intensity is closely related to the size and number of cavitation events. However, the mechanistic origins of bubbles constituting vortex cavitation remains unclear, although it has been concluded that the pressure fields generated by the cavitation collapse strongly depends on the bubble geometry. The common view is that vortex cavitation consists of numerous small spherical bubbles. In the present paper, aspects of vortex cavitation arising in a Venturi tube were visualized using high-speed X-ray imaging at SPring-8 and European XFEL. It was discovered that vortex cavitation in a Venturi tube consisted of angulated rather than spherical bubbles. The tangential velocity of the surface of vortex cavitation was assessed considering the Rankine vortex model.	Dec 2023
	Laser-induced, single droplet fragmentation dynamics revealed through megahertz x-ray microscopy Fabian Reuter , Tokushi Sato , Valerio Bellucci , Sarlota Birnsteinova , Carsten Deiter , Jayanath C. P. Koliyadu , Romain Letrun , Pablo Villanueva-Perez , Richard Bean , Adrian P. Mancuso , Alke Meents , Patrik Vagovic , Claus-Dieter Ohl Physics Of Fluids 35 DOI: 10.1063/5.0171225 Open Access Show Abstract ▼ Abstract: The fragmentation dynamics of single water droplets from laser irradiation is studied with megahertz frame rate x-ray microscopy. Owed to the nearly refraction-free and penetrating imaging technique, we could look into the interior of the droplet and reveal that two mechanisms are responsible for the initial explosive fragmentation of the droplet. First, reflection and diffraction of the laser beam at the droplet interface result in the formation of laser ray caustics that lead to non-homogeneous heating of the droplet, locally above the critical temperature. Second, homogeneous cavitation in the droplet that is likely caused from shockwaves reflected as tension waves at the acoustic soft boundaries of the droplet. Further atomization occurs in three stages, first a fine sub-micrometer sized mist forms on the side of the droplet posterior to laser incidence, then micrometer sized droplets are expelled from the rim of an expanding liquid sheet, and finally into droplets of larger size through hole and ligament formation in the thinning liquid sheet where ligaments pinch off.	Nov 2023
I03-Macromolecular Crystallography	Megahertz serial crystallography Max O. Wiedorn , Dominik Oberthuer , Richard Bean , Robin Schubert , Nadine Werner , Brian Abbey , Martin Aepfelbacher , Luigi Adriano , Aschkan Allahgholi , Nasser Al-Qudami , Jakob Andreasson , Steve Aplin , Salah Awel , Kartik Ayyer , Saša Bajt , Imrich Barák , Sadia Bari , Johan Bielecki , Sabine Botha , Djelloul Boukhelef , Wolfgang Brehm , Sandor Brockhauser , Igor Cheviakov , Matthew A. Coleman , Francisco Cruz-Mazo , Cyril Danilevski , Connie Darmanin , R. Bruce Doak , Martin Domaracky , Katerina Dörner , Yang Du , Hans Fangohr , Holger Fleckenstein , Matthias Frank , Petra Fromme , Alfonso M. Gañán-Calvo , Yaroslav Gevorkov , Klaus Giewekemeyer , Helen Mary Ginn , Heinz Graafsma , Rita Graceffa , Dominic Greiffenberg , Lars Gumprecht , Peter Göttlicher , Janos Hajdu , Steffen Hauf , Michael Heymann , Susannah Holmes , Daniel A. Horke , Mark S. Hunter , Siegfried Imlau , Alexander Kaukher , Yoonhee Kim , Alexander Klyuev , Juraj Knoška , Bostjan Kobe , Manuela Kuhn , Christopher Kupitz , Jochen Küpper , Janine Mia Lahey-Rudolph , Torsten Laurus , Karoline Le Cong , Romain Letrun , P. Lourdu Xavier , Luis Maia , Filipe R. N. C. Maia , Valerio Mariani , Marc Messerschmidt , Markus Metz , Davide Mezza , Thomas Michelat , Grant Mills , Diana C. F. Monteiro , Andrew Morgan , Kerstin Mühlig , Anna Munke , Astrid Münnich , Julia Nette , Keith A. Nugent , Theresa Nuguid , Allen M. Orville , Suraj Pandey , Gisel Pena , Pablo Villanueva-Perez , Jennifer Poehlsen , Gianpietro Previtali , Lars Redecke , Winnie Maria Riekehr , Holger Rohde , Adam Round , Tatiana Safenreiter , Iosifina Sarrou , Tokushi Sato , Marius Schmidt , Bernd Schmitt , Robert Schönherr , Joachim Schulz , Jonas A. Sellberg , M. Marvin Seibert , Carolin Seuring , Megan L. Shelby , Robert L. Shoeman , Marcin Sikorski , Alessandro Silenzi , Claudiu A. Stan , Xintian Shi , Stephan Stern , Jola Sztuk-Dambietz , Janusz Szuba , Aleksandra Tolstikova , Martin Trebbin , Ulrich Trunk , Patrik Vagovic , Thomas Ve , Britta Weinhausen , Thomas A. White , Krzysztof Wrona , Chen Xu , Oleksandr Yefanov , Nadia Zatsepin , Jiaguo Zhang , Markus Perbandt , Adrian P. Mancuso , Christian Betzel , Henry Chapman , Anton Barty Nature Communications 9 DOI: 10.1038/s41467-018-06156-7 Open Access Show Abstract ▼ Abstract: The new European X-ray Free-Electron Laser is the first X-ray free-electron laser capable of delivering X-ray pulses with a megahertz inter-pulse spacing, more than four orders of magnitude higher than previously possible. However, to date, it has been unclear whether it would indeed be possible to measure high-quality diffraction data at megahertz pulse repetition rates. Here, we show that high-quality structures can indeed be obtained using currently available operating conditions at the European XFEL. We present two complete data sets, one from the well-known model system lysozyme and the other from a so far unknown complex of a β-lactamase from K. pneumoniae involved in antibiotic resistance. This result opens up megahertz serial femtosecond crystallography (SFX) as a tool for reliable structure determination, substrate screening and the efficient measurement of the evolution and dynamics of molecular structures using megahertz repetition rate pulses available at this new class of X-ray laser source.	Oct 2018

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