16 research outputs found
Online dynamic flat-field correction for MHz Microscopy data at European XFEL
The X-ray microscopy technique at the European X-ray free-electron laser
(EuXFEL), operating at a MHz repetition rate, provides superior contrast and
spatial-temporal resolution compared to typical microscopy techniques at other
X-ray sources. In both online visualization and offline data analysis for
microscopy experiments, baseline normalization is essential for further
processing steps such as phase retrieval and modal decomposition. In addition,
access to normalized projections during data acquisition can play an important
role in decision-making and improve the quality of the data. However, the
stochastic nature of XFEL sources hinders the use of existing flat-flied
normalization methods during MHz X-ray microscopy experiments. Here, we present
an online dynamic flat-field correction method based on principal component
analysis of dynamically evolving flat-field images. The method is used for the
normalization of individual X-ray projections and has been implemented as an
online analysis tool at the Single Particles, Clusters, and Biomolecules and
Serial Femtosecond Crystallography (SPB/SFX) instrument of EuXFEL.Comment: 14 pages, 7 figure
Ultrasound cavitation and exfoliation dynamics of 2D materials re-vealed in operando by X-ray free electron laser megahertz imaging
Ultrasonic liquid phase exfoliation is a promising method for the production
of two-dimensional (2D) layered materials. A large number of studies have been
made in investigating the underlying ultrasound exfoliation mechanisms.
However, due to the experimental challenges for capturing the highly transient
and dynamic phenomena in real-time at sub-microsecond time and micrometer
length scales simultaneously, most theories reported to date still remain
elusive. Here, using the ultra-short X-ray Free Electron Laser pulses (~25ps)
with a unique pulse train structure, we applied MHz X-ray Microscopy and
machine-learning technique to reveal unambiguously the full cycles of the
ultrasound cavitation and graphite layer exfoliation dynamics with
sub-microsecond and micrometer resolution. Cyclic fatigue shock wave impacts
produced by ultrasound cloud implosion were identified as the dominant
mechanism to deflect and exfoliate graphite layers mechanically. For the
graphite flakes, exfoliation rate as high as ~5 angstroms per shock wave impact
was observed. For the HOPG graphite, the highest exfoliation rate was ~0.15
angstroms per impact. These new findings are scientifically and technologically
important for developing industrial upscaling strategies for ultrasonic
exfoliation of 2D materials
First operation of the JUNGFRAU detector in 16-memory cell mode at European XFEL
The JUNGFRAU detector is a well-established hybrid pixel detector developed at the Paul Scherrer Institut (PSI) designed for free-electron laser (FEL) applications. JUNGFRAU features a charge-integrating dynamic gain switching architecture, with three different gain stages and 75 μm pixel pitch. It is widely used at the European X-ray Free-Electron Laser (EuXFEL), a facility which produces high brilliance X-ray pulses at MHz repetition rate in the form of bursts repeating at 10 Hz. In nominal configuration, the detector utilizes only a single memory cell and supports data acquisition up to 2 kHz. This constrains the operation of the detector to a 10 Hz frame rate when combined with the pulsed train structure of the EuXFEL. When configured in so-called burst mode, the JUNGFRAU detector can acquire a series of images into sixteen memory cells at a maximum rate of around 150 kHz. This acquisition scheme is better suited for the time structure of the X-rays as well as the pump laser pulses at the EuXFEL. To ensure confidence in the use of the burst mode at EuXFEL, a wide range of measurements have been performed to characterize the detector, especially to validate the detector alibration procedures. In particular, by analyzing the detector response to varying photon intensity (so called ‘intensity scan’), special attention was given to the characterization of the transitions between gain stages. The detector was operated in both dynamic gain switching and fixed gain modes. Results of these measurements indicate difficulties in the characterization of the detector dynamic gain switching response while operated in burst mode, while no major issues have been found with fixed gain operation. Based on this outcome, fixed gain operation mode with all the memory cells was used during two experiments at EuXFEL, namely in serial femtosecond protein crystallography and Kossel lines measurements. The positive outcome of these two experiments validates the good results previously obtained, and opens the possibility for a wider usage of the detector in burst operation mode, although compromises are needed on the dynamic range
Observation of substrate diffusion and ligand binding in enzyme crystals using high-repetition-rate mix-and-inject serial crystallography
18 pags, 11 figs, 5 tabsHere, we illustrate what happens inside the catalytic cleft of an enzyme when substrate or ligand binds on single-millisecond timescales. The initial phase of the enzymatic cycle is observed with near-atomic resolution using the most advanced X-ray source currently available: the European XFEL (EuXFEL). The high repetition rate of the EuXFEL combined with our mix-and-inject technology enables the initial phase of ceftriaxone binding to the Mycobacterium tuberculosis β-lactamase to be followed using time-resolved crystallography in real time. It is shown how a diffusion coefficient in enzyme crystals can be derived directly from the X-ray data, enabling the determination of ligand and enzyme-ligand concentrations at any position in the crystal volume as a function of time. In addition, the structure of the irreversible inhibitor sulbactam bound to the enzyme at a 66 ms time delay after mixing is described. This demonstrates that the EuXFEL can be used as an important tool for biomedically relevant research.This work was supported by the National Science Foundation Science and Technology Center 'BioXFEL' through award STC-1231306, and in part by the US Department of Energy, Office of Science, Basic Energy Sciences under contract DESC0002164 (AO, algorithm design and development) and by the National Science Foundation under contract Nos. 1551489 (AO, underlying analytical models) and DBI-2029533 (AO, functional conformations). This material is based upon work supported by the National Science Foundation Graduate Research Fellowship Program under Grant No. 1450681 to JLO. The work was also supported by funds from the National Institutes of Health grant R01 GM117342-0404. Funding and support are also acknowledged from the National Institutes of Health grant R01 GM095583, from the Biodesign Center for Applied Structural Discovery at ASU, from National Science Foundation award No. 1565180 and the US Department of Energy through Lawrence Livermore National Laboratory under contract DE-AC52-07NA27344. KAZ was supported by the Cornell Molecular Biophysics Training Program (NIH T32-GM008267). This work was also supported by the Cluster of Excellence 'CUI: Advanced Imaging of Matter' of the Deutsche Forschungsgemeinschaft (DFG), EXC 2056, project ID 390715994. CFEL is supported by the Gottfried Wilhelm Leibniz Program of the DFG, the 'X-probe' project funded by the European Union 2020 Research and Innovation Program under Marie Sklodowska-Curie grant agreement 637295, the European Research Council, 'Frontiers in Attosecond X-ray Science: Imaging and Spectroscopy (AXSIS)', ERC-2013-SyG 609920, and the Human Frontiers Science Program grant RGP0010 2017. This work is also supported by the AXSIS project funded by the European Research Council under the European Union Seventh Framework Program (FP/2007-2013)/ERC Grant Agreement No. 609920.Peer reviewe
High-harmonic generation wave front dependence on a driving infrared wave front
With high-harmonic generation (HHG), spatially and temporally coherent XUV to soft x-ray (100 nm to 10 nm)table-top sources can be realized by focusing a driving infrared (IR) laser on a gas target. For applications such ascoherent diffraction imaging, holography, plasma diagnostics, or pump–probe experiments, it is desirable to havecontrol over the wave front (WF) of the HHs to maximize the number of XUV photons on target or to tailor the WF.Here, we demonstrate control of the XUV WF by tailoring the driving IR WF with a deformable mirror. The WFsof both IR and XUV beams are monitored with WF sensors. We present a systematic study of the dependence of theaberrations of the HHs on the aberrations of the driving IR laser and explain the observations with propagationsimulations. We show that we can control the astigmatism of the HHs by changing the astigmatism of the drivingIR laser without compromising the HH generation efficiency with a WF quality fromλ/8 toλ/13.3. This allows usto shape the XUV beam without changing any XUV optical element
3D atomic structure from a single X-ray free electron laser pulse
Abstract X-ray Free Electron Lasers (XFEL) are cutting-edge pulsed x-ray sources, whose extraordinary pulse parameters promise to unlock unique applications. Several new methods have been developed at XFELs; however, no methods are known, which allow ab initio atomic level structure determination using only a single XFEL pulse. Here, we present experimental results, demonstrating the determination of the 3D atomic structure from data obtained during a single 25 fs XFEL pulse. Parallel measurement of hundreds of Bragg reflections was done by collecting Kossel line patterns of GaAs and GaP. To the best of our knowledge with these measurements, we reached the ultimate temporal limit of the x-ray structure solution possible today. These measurements open the way for obtaining crystalline structures during non-repeatable fast processes, such as structural transformations. For example, the atomic structure of matter at extremely non-ambient conditions or transient structures formed in irreversible physical, chemical, or biological processes may be captured in a single shot measurement during the transformation. It would also facilitate time resolved pump-probe structural studies making them significantly shorter than traditional serial crystallography
High numerical aperture Hartmann wave front sensor for extreme ultraviolet spectral range
International audienc
Online dynamic flat-field correction for MHz microscopy data at European XFEL
The high pulse intensity and repetition rate of the European X-ray Free-Electron Laser (EuXFEL) provide superior temporal resolution compared with other X-ray sources. In combination with MHz X-ray microscopy techniques, it offers a unique opportunity to achieve superior contrast and spatial resolution in applications demanding high temporal resolution. In both live visualization and offline data analysis for microscopy experiments, baseline normalization is essential for further processing steps such as phase retrieval and modal decomposition. In addition, access to normalized projections during data acquisition can play an important role in decision-making and improve the quality of the data. However, the stochastic nature of X-ray free-electron laser sources hinders the use of standard flat-field normalization methods during MHz X-ray microscopy experiments. Here, an online (i.e. near real-time) dynamic flat-field correction method based on principal component analysis of dynamically evolving flat-field images is presented. The method is used for the normalization of individual X-ray projections and has been implemented as a near real-time analysis tool at the Single Particles, Clusters, and Biomolecules and Serial Femtosecond Crystallography (SPB/SFX) instrument of EuXFEL
Enhancement and maximum in the isobaric specific-heat capacity measurements of deeply supercooled water using ultrafast calorimetry
Knowledge of the temperature dependence of the isobaric specific heat (Cp) upon deep supercooling can give insights regarding the anomalous properties of water. If a maximum in Cp exists at a specific temperature, as in the isothermal compressibility, it would further validate the liquid-liquid critical point model that can explain the anomalous increase in thermodynamic response functions. The challenge is that the relevant temperature range falls in the region where ice crystallization becomes rapid, which has previously excluded experiments. Here, we have utilized a methodology of ultrafast calorimetry by determining the temperature jump from femtosecond X-ray pulses after heating with an infrared laser pulse and with a sufficiently long time delay between the pulses to allow measurements at constant pressure. Evaporative cooling of ∼15-μm diameter droplets in vacuum enabled us to reach a temperature down to ∼228 K with a small fraction of the droplets remaining unfrozen. We observed a sharp increase in Cp, from 88 J/mol/K at 244 K to about 218 J/mol/K at 229 K where a maximum is seen. The Cp maximum is at a similar temperature as the maxima of the isothermal compressibility and correlation length. From the Cp measurement, we estimated the excess entropy and self-diffusion coefficient of water and these properties decrease rapidly below 235 K.QC 20220317</p