Mosaic Crystals Research Articles

Observation of the orientation of membrane protein crystals grown in high magnetic force fields

Crystallization of membrane proteins in magnetic fields is thought to reveal the magnetic orientations of crystals, and is expected to enhance crystal quality for X-ray crystallographic analysis. The light-harvesting complex 2 (LH2) from a photosynthetic bacterium, Thermochromatium tepidum was crystallized in steep-gradient magnetic fields. The rod-shaped crystals of LH2 grown in the magnetic fields were oriented parallel to the magnetic field direction. An X-ray diffraction experiment indicated that the overall R value and crystal mosaicity are improved for the magnetically oriented crystal, and the helix bundles of LH2 were located parallel to the magnetic field direction in the crystal packing.

Multilayer laser-assisted deposition on single crystal superalloy substrates

Laser powder deposition is a promising method for repairing single crystal Ni-based superalloy components used in the hot section of gas turbine engines. In this paper, recent results on multilayer deposits of NiCrAlY and Rene N4 on (100) single crystal substrates of SRR99- and CMSX-4 Ni-based superalloys are summarised. The deposited material presents a columnar dendritic microstructure consisting of arrays of similarly oriented dendrites forming a mosaic single crystal. Since solidification is epitaxial, the deposits inherit the orientation of the substrate. After aging, the �� '-Ni3Al precipitates do not present the cuboid shape required for high-temperature strength owing to chemical segregation within the dendrite arms resulting from solidification solute partition. Heat treatments capable of creating the proper particle microstructures were devised.

Imaging and diffraction of protein crystallization using TEM

Structural biology relies on good-quality protein crystals in order for structure determination. Many factors affect the growth process of a protein crystal including the way it nucleates and the types of damage and contamination during its growth. Although the nucleation process and quality of a crystal is vital to structure determination, they are both under-studied areas of research. Our research begins to explore ways of measuring the quality of protein crystals, using TEM, thus overcoming the problems associated with viewing wet specimens in a vacuum. Our current understanding of nucleation is that it is a two-step mechanism involving the formation of nuclei from dense liquid clusters; however; it is still unclear whether nuclei first start as amorphous aggregates or as crystalline lattices. Potentially, electron diffraction may be capable of uncovering this process. Using TEM imaging and diffraction of lysozyme as a model protein crystal, we report the internal two-dimensional strain and the density of crystallites in a protein crystal, at a resolution never seen before. The TEM diffraction shows unique features of crystal mosaicity that can be directly correlated to TEM images.

Estimation of microblock sizes in mosaic crystals according to fast electron radiation characteristics

The possibilities of a previously proposed technique for determining the characteristic sizes of microblocks in mosaic aα-class crystals have been analyzed. Determination is performed according to the ratio between the measured and calculated values for the diffraction suppression of the fixed-energy bremsstrahlung yield. The limits of applicability of the technique have been revealed. It is demonstrated that the technique can be implemented in an electron accelerator with the average energy Ee ∼ 30–40 MeV and long baselines making it possible to use crystal-diffraction spectrometers. The influence of microblock sizes on coherent electromagnetic processes in real crystals is discussed.

Time-of-flight studies of multiple Bragg reflections in cylindrically bent perfect crystals

Multiple Bragg reflections (MBRs) realized in a bent perfect crystal (BPC) slab by sets of different lattice planes behave differently from the case of perfect nondeformed or mosaic crystals. Because of elastic bending (homogeneous deformation), individual sets of lattice planes are mutually in dispersive diffraction geometry and the kinematical approach can be applied on this MBR process. The elastic deformation produced by the cylindrical bending can enormously strengthen the MBR effects, which can then be investigated even at small neutron sources. By using neutron diffraction and the time-of-flight method, carried out at the 45 MeV linac-based pulsed cold neutron source at Hokkaido University, it has been demonstrated that when setting the BPC slabs in the symmetric transmission geometry many strong MBRs accompanying forbidden Si(222) or Si(002) reflections can be observed. The advantage of the time-of-flight method consists in the fact that it is possible to observe not only primary MBRs related to the basic forbidden reflections but also their higher orders, which could be easily separated in the time-of-flight spectra.

Focal aberrations of large-aperture HOPG von-Hàmos x-ray spectrometers

Focal aberrations of large-aperture highly oriented pyrolytic graphite (HOPG) crystals in von-Hàmos geometry are investigated by experimental and computational methods. A mosaic HOPG crystal film of 100 μm thickness diffracts 8 keV x-rays. This thickness is smaller than the absorption depth of the symmetric 004-reflection, which amounts to 257 μm. Cylindrically bent crystals with 110mm radius of curvature and up to 100 mm collection width produce a X-shaped halo around the focus. This feature vanishes when the collection aperture is reduced, but axial spectral profiles show that the resolution is not affected. X-ray topography reveals significant inhomogeneous crystallite domains of 2±1mm diameter along the entire crystal. Rocking curves shift by about ±20arcmin between domains, while their full width at half-maximum varies between 30 and 50 arcmin. These inhomogeneities are not imprinted at the focal spot, since the monochromatically reflecting area of the crystal is large compared to inhomogeneities. Ray-tracing calculations using a Monte-Carlo-based algorithm developed for mosaic crystals reproduce the X-shaped halo in the focal plane, stemming from the mosaic defocussing in the non-dispersive direction in combination with large apertures. The best achievable resolution is found by analyzing a diversity of rocking curve widths, source sizes and crystal thicknesses for 8 keV x-rays to be ΔE/E ∼ 10−4. Finally a general analytic expression for the shape of the aberration is derived.

Preparation of bent crystals as high-efficiency optical elements for hard x-ray astronomy

Curved crystals, instead of flat mosaic crystals, can be used as optical elements of a Laue lens for hard x- and gamma-ray astronomy to increase the diffraction efficiency. We propose to achieve the bending of the crystals by a controlled surface damaging, which introduces defects in a layer of few tens nanometers in thickness undergoing a highly compressive strain. Several oriented silicon and gallium arsenide wafer crystals have been treated. The local and mean curvature radii of each sample have been determined by means of high resolution x-ray diffraction measurements in Bragg condition at low energy (8 keV). Silicon samples showed spherical curvatures, whereas GaAs-treated samples evidenced elliptical curvatures with major axes corresponding to the 〈110〉 crystallographic directions. Curvature radii between 3 and 70 m were easily obtained in wafers of different thicknesses. The characterization of GaAs samples performed in Laue geometry at gamma-ray energy of 120 keV confirmed the increase of the diffraction efficiency in the bent crystals.

Estimation of grains size in mosaic crystals by means of radiation of fast electrons in these samples

There were analyzed the possibilities of the previously suggested method for determining the characteristic dimensions of grains in mosaic crystals of diffraction suppression of yield of the bremsstrahlung with the fixed energy and calculated results. There were defined the bounds of the method applicability and also there were taken into account more accurately the effect of the absorption process of X-rays on the reflectivity.

High-resolution x-ray characterization of mosaic crystals for hard x-ray astronomy

GaAs, Cu, CdTe, and CdZnTe crystals have been studied as optical elements for lenses for hard x-ray astronomy. High-resolution x-ray diffraction at 8 keV in Bragg geometry and at synchrotron at energies up to 500 keV in Laue geometry has been used. A good agreement was found between the mosaicity evaluated in Bragg geometry at 8 keV with x-ray penetration of the order of few tens of micrometers and that derived at synchrotron in transmission Laue geometry at higher x-ray energies. Mosaicity values in a range between a few to 150 arcsec were found in all the samples but, due to the presence of crystal grains in the cm range, CdTe and CdZnTe crystals were found not suitable. Cu crystals exhibit a mosaicity of the order of several arcmin; they indeed were found to be severely affected by cutting damage which could only be removed with a very deep etching. The full width at half maximum of the diffraction peaks decreased at higher x-ray energies showing that the peak broadening is affected by crystallite size. GaAs crystals grown by Czochralski method showed a mosaic spread up to 30 arcsec and good diffraction efficiency up to energies of 500 keV. The use of thermal treatments as a possible method to increase the mosaic spread was also evaluated.

Coherent acoustic wave oscillations and melting on Ag(111) surface by time resolved x-ray diffraction

The transient structural disorder on the Ag(111) crystal after excitation with fs pulses was studied by means of time resolved x-ray diffraction. The lattice disorder after UV irradiation is detected by changes in the XRD rocking curve including peak shift, broadening, and total diffraction intensity. We have observed blast and pressure wave formation and melting and mosaic crystal formation during re-crystallization. A blast force was formed within 2 ps after fs UV irradiation of the crystal, followed lattice contraction, melting phase transition, and mosaic crystal formation as the temperature decreases below melting. The experimental data are also supported by theoretical simulations.

Evaluation of freestanding boron-doped diamond grown by chemical vapour deposition as substrates for vertical power electronic devices

In this study, 4 × 4 mm2 freestanding boron-doped diamond single crystals with thickness up to 260 μm have been fabricated by plasma assisted chemical vapour deposition. The boron concentrations measured by secondary ion mass spectroscopy were 1018 to 1020 cm−3 which is in a good agreement with the values calculated from Fourier transform infrared spectroscopy analysis, thus indicating that almost all incorporated boron is electrically active. The dependence of lattice parameters and crystal mosaicity on boron concentrations have also been extracted from high resolution x-ray diffraction experiments on (004) planes. The widths of x-ray rocking curves have globally shown the high quality of the material despite a substantial broadening of the peak, indicating a decrease of structural quality with increasing boron doping levels. Finally, the suitability of these crystals for the development of vertical power electronic devices has been confirmed by four-point probe measurements from which electrical resistivities as low as 0.26 Ω cm have been obtained.

Investigation of multiple Bragg reflections at a constant neutron wavelength and their possible separation

Multiple Bragg reflections (MBR) realized in one bent-perfect crystal (BPC) slab by sets of different lattice planes behave differently in comparison to the case of perfect nondeformed or mosaic crystal. Individual sets of lattice planes are mutually in dispersive diffraction geometry and the kinematical approach can be applied on this MBR process. It has been found that contrary to the perfect nondeformed or mosaic crystal, individual reflections participating in the MBR process can be spatially separated.

Optimal fine ϕ-slicing for single-photon-counting pixel detectors

The data-collection parameters used in a macromolecular diffraction experiment have a strong impact on data quality. A careful choice of parameters leads to better data and can make the difference between success and failure in phasing attempts, and will also result in a more accurate atomic model. The selection of parameters has to account for the application of the data in various phasing methods or high-resolution refinement. Furthermore, experimental factors such as crystal characteristics, available experiment time and the properties of the X-ray source and detector have to be considered. For many years, CCD detectors have been the prevalent type of detectors used in macromolecular crystallography. Recently, hybrid pixel X-ray detectors that operate in single-photon-counting mode have become available. These detectors have fundamentally different characteristics compared with CCD detectors and different data-collection strategies should be applied. Fine φ-slicing is a strategy that is particularly well suited to hybrid pixel detectors because of the fast readout time and the absence of readout noise. A large number of data sets were systematically collected from crystals of four different proteins in order to investigate the benefit of fine φ-slicing on data quality with a noise-free detector. The results show that fine φ-slicing can substantially improve scaling statistics and anomalous signal provided that the rotation angle is comparable to half the crystal mosaicity.

Proposal for a Laue lens with quasi-mosaic crystalline tiles

Quasi-mosaicity is an effect of secondary bending within a crystal driven by crystalline anisotropy. This effect can be used to fabricate a series of curved crystals for the realization of a Laue lens. It is highlighted that crystals bent by the quasi-mosaic effect allow very high resolution focusing with respect to mosaic crystals. Under the same conditions for energy passband, crystal size and flux of incident photons, a Laue lens based on quasi-mosaic crystals would increase the signal-to-noise ratio by about an order of magnitude compared to the same lens with mosaic crystals. Moreover, no mosaic defocusing occurs for quasi-mosaic crystals.

Optimal fine ϕ slicing for single photon counting pixel detectors

The data-collection parameters used in a macromolecular diffraction experiment have a strong impact on data quality. A careful choice of parameters leads to better data and can make the difference between success and failure in phasing attempts, and will also result in a more accurate atomic model. The selection of parameters has to account for the application of the data in various phasing methods or high-resolution refinement. Furthermore, experimental factors such as crystal characteristics, available experiment time and the properties of the X-ray source and detector have to be considered. For many years, CCD detectors have been the prevalent type of detectors used in macromolecular crystallography. Recently, hybrid pixel X-ray detectors that operate in single-photon-counting mode have become available. These detectors have fundamentally different characteristics compared with CCD detectors and different data-collection strategies should be applied. Fine φ-slicing is a strategy that is particularly well suited to hybrid pixel detectors because of the fast readout time and the absence of readout noise. A large number of data sets were systematically collected from crystals of four different proteins in order to investigate the benefit of fine φ-­slicing on data quality with a noise-free detector. The results show that fine φ-slicing can substantially improve scaling statistics and anomalous signal provided that the rotation angle is comparable to half the crystal mosaicity.

Cold neutron scattering in imperfect deuterium crystals

The cross sections for cold neutron scattering in mosaic deuterium crystals have been calculated for various target structures. The theoretical results are compared with the recent experimental data obtained at the Paul Scherrer Institute (PSI) with the use of FUNSPIN beamline. It is shown that various patterns of the Bragg cross sections, which were observed in different solid D 2 samples at the same temperature, can be explained by contributions from a limited number of monocrystal orientations and the mosaic spread of about 3 degrees.

Crystalline perfection of an aluminium single crystal determined by neutron diffraction

In this work, a study of the crystalline perfection of an aluminium single crystal is presented. The study shows that, from three-dimensional neutron diffraction rocking curves, it is possible to characterize the individual crystalline domains of a multidomain crystal. From a macroscopic point of view, the determination of the domains allows an evaluation of the crystalline perfection of the crystal under study. Three-dimensional rocking curves have been obtained by neutron diffraction from a large mosaic aluminium crystal. Construction of a contour map of individual domains made it easier to determine the breadth and relative intensity of each domain. The angular distances between domains were also determined.

Optimum velocity of a phase-space transformer for cold-neutron backscattering spectroscopy

Cold-neutron backscattering spectrometers are designed for inelastic neutron scattering experiments at a high energy resolution, where 0.5 µeV FWHM can routinely be achieved at the incident wavelength λ ≃ 6.3 Å. The phase-space transformation (PST) technique can be used to enhance the neutron flux at the sample position of such backscattering spectrometers at the expense of an acceptable increase of the beam divergence. Technically, the PST is achieved by a rotating disc carrying mosaic crystals on its circumference. Here a new analytical framework to describe the Bragg reflection of a divergent polychromatic beam from a moving mosaic crystal is discussed. Results obtained using this framework are compared with detailed Monte Carlo numerical simulations. The results presented here provide a deeper understanding of the PST and in particular of the optimum circumferential crystal speed of a PST device.

Parabolic versus elliptic focusing – Optimization of the focusing design of a cold triple-axis neutron spectrometer by Monte-Carlo simulations

We present Monte-Carlo simulations for the focusing design of a novel cold-neutron triple-axis spectrometer to be installed at the end position of the cold guide NL-1 of the research reactor FRM-II in Munich, Germany. Our simulations are of general relevance for the design of triple-axis spectrometers at end positions of neutron guides. Using the McStas program code we performed ray trajectories to compare parabolic and elliptic focusing concepts. In addition the design of the monochromator was optimized concerning crystal size and mosaic spread. The parabolic focusing concept is superior to the elliptic alternative in view of the neutron intensity distribution as a function of energy and divergence. In particular, the elliptical configuration leads to an inhomogeneous divergence distribution.

Influence of crystal mosaicity on the X-radiation characteristics observed at a small angle to the particle velocity direction

The experimentally measured yields of X-rays generated by 500-MeV electrons (the X-ray energies are ω ∼ γωp) in oriented tungsten single crystals are analyzed. A series of experiments have been performed at the Tomsk synchrotron with the use of crystal-diffraction spectrometers based on mosaic pyrolytic graphite crystals. The measured results are shown to be explained by competition between parametric X-radiation and bremsstrahlung diffraction in mosaic crystals of the aα class. The characteristic sizes of microblocks of refractory metal crystals are discussed from the standpoint of their influence on the positron yield in designed positron sources. A method for determining the characteristic sizes of microblocks in mosaic crystals of the aα class is proposed.