您现在的位置:首页>美国卫生研究院文献>Acta Crystallographica. Section A, Foundations and Advances

期刊信息

  • 期刊名称:

    -

  • 刊频: Bimonthly
  • NLM标题: Acta Crystallogr A Found Adv
  • iso缩写: -
  • ISSN: -

年度选择

更多>>

  • 排序:
  • 显示:
  • 每页:
全选(0
<1/4>
69条结果
  • 机译 XGANDALF –用于晶格寻找的扩展梯度下降算法
    摘要:Serial crystallography records still diffraction patterns from single, randomly oriented crystals, then merges data from hundreds or thousands of them to form a complete data set. To process the data, the diffraction patterns must first be indexed, equivalent to determining the orientation of each crystal. A novel automatic indexing algorithm is presented, which in tests usually gives significantly higher indexing rates than alternative programs currently available for this task. The algorithm does not require prior knowledge of the lattice parameters but can make use of that information if provided, and also allows indexing of diffraction patterns generated by several crystals in the beam. Cases with a small number of Bragg spots per pattern appear to particularly benefit from the new approach. The algorithm has been implemented and optimized for fast execution, making it suitable for real-time feedback during serial crystallography experiments. It is implemented in an open-source C++ library and distributed under the LGPLv3 licence. An interface to it has been added to the CrystFEL software suite.
  • 机译 X射线衍射莫尔条纹特性的理论研究。二。角度整合的莫尔图像的插图
    • 作者:Jun-ichi Yoshimura
    • 刊名:Acta Crystallographica. Section A, Foundations and Advances
    • 2019年第Pt 4期
    摘要:Using a theory of X-ray diffraction moiré fringes developed in a previous paper, labelled Part I [Yoshimura (2015). Acta Cryst. A71, 368–381], the X-ray moiré images of a silicon bicrystal having a weak curvature strain and an interspacing gap, assumed to be integrated for an incident-wave angular width, are simulation-computed over a wide range of crystal thicknesses and incident-wave angular width, likely under practical experimental conditions. Along with the simulated moiré images, the graphs of characteristic quantities on the moiré images are presented for a full understanding of them. The treated moiré images are all of rotation moiré. Mo Kα1 radiation and the 220 reflection were assumed in the simulation. The results of this simulation show that fringe patterns, which are significantly modified from simple straight fringes of rotation moiré, appear in some ranges of crystal thicknesses and incident-wave angular width, due to a combined effect of Pendellösung oscillation and an added phase difference from the interspacing gap, under the presence of a curvature strain. The moiré fringes which slope to the perpendicular direction to the diffraction vector in spite of the assumed condition of rotation moiré, and fringe patterns where low-contrast bands are produced with a sharp bend of fringes arising along the bands are examples of the modified fringe pattern. This simulation study provides a wide theoretical survey of the type of bicrystal moiré image produced under a particular condition.
  • 机译 实验获得的计算机模拟的X射线非对称八光束针孔地形图
    摘要:In this study, experimentally obtained eight-beam pinhole topographs for a silicon crystal using synchrotron X-rays were compared with computer-simulated images, and were found to be in good agreement. The experiment was performed with an asymmetric all-Laue geometry. However, the X-rays exited from both the bottom and side surfaces of the crystal. The simulations were performed using two different approaches: one was the integration of the n-beam Takagi–Taupin equation, and the second was the fast Fourier transformation of the X-ray amplitudes obtained by solving the eigenvalue problem of the n-beam Ewald–Laue theory as reported by Kohn & Khikhlukha [Acta Cryst. (2016), A72, 349–356] and Kohn [Acta Cryst. (2017), A73, 30–38].
  • 机译 十二边形准晶体的完整实空间分析
    摘要:The atomically resolved real-space structure of a long-range-ordered dodecagonal quasicrystal is determined based on scanning tunnelling microscopy. For the BaTiO3-derived oxide quasicrystal which spontaneously forms on a Pt(111) surface, 8100 atomic positions have been determined and are compared with an ideal Niizeki–Gähler tiling. Although the Niizeki–Gähler tiling has a complex three-element structure, the abundance of the triangle, square and rhomb tiling elements in the experimental data closely resembles the ideal frequencies. Similarly, the frequencies of all possible next-neighbour tiling combinations are, within the experimental uncertainty, identical to the ideal tiling. The angular and orientational distributions of all individual tiling elements show the characteristics of the dodecagonal quasicrystal. In contrast, the analysis of the orientation of characteristic and more complex tiling combinations indicates the partial decomposition of the quasicrystal into small patches with locally reduced symmetry. These, however, preserve the long-range quasicrystal coherence. The symmetry reduction from dodecagonal to sixfold is assigned to local interaction with the threefold substrate. It leads to atomic flips which preserve the number of quasicrystal tiling elements.
  • 机译 金属间化合物中弱序畴的原理:Fe2Al5中原子堆积和电子的协同效应
    摘要:Many complex intermetallic structures feature a curious juxtaposition of domains with strict 3D periodicity and regions of much weaker order or incommensurability. This article explores the basic principles leading to such arrangements through an investigation of the weakly ordered channels of Fe2Al5. It starts by experimentally confirming the earlier crystallographic model of the high-temperature form, in which nearly continuous columns of electron density corresponding to disordered Al atoms emerge. Then electronic structure calculations on ordered models are used to determine the factors leading to the formation of these columns. These calculations reveal electronic pseudogaps near 16 electrons/Fe atom, an electron concentration close to the Al-rich side of the phase’s homogeneity range. Through a reversed approximation Molecular Orbital (raMO) analysis, these pseudogaps are correlated with the filling of 18-electron configurations on the Fe atoms with the support of isolobal σ Fe–Fe bonds. The resulting preference for 16 electrons/Fe requires a fractional number of Al atoms in the Fe2Al5 unit cell. Density functional theory–chemical pressure (DFT-CP) analysis is then applied to investigate how this nonstoichiometry is accommodated. The CP schemes reveal strong quadrupolar distributions on the Al atoms of the channels, suggestive of soft atomic motions along the undulating electron density observed in the Fourier map that allow the Al positions to shift easily in response to compositional changes. Such a combination of preferred electron counts tied to stoichiometry and continuous paths of CP quadrupoles could provide predictive indicators for the emergence of channels of disordered or incommensurately spaced atoms in intermetallic structures.
  • 机译 W / Si多层膜中相关横向密度波动的掠入射小角X射线散射研究
    摘要:A structural characterization of W/Si multilayers using X-ray reflectivity (XRR), scanning transmission electron microscopy (STEM) and grazing-incidence small-angle X-ray scattering (GISAXS) is presented. STEM images revealed lateral, periodic density fluctuations in the Si layers, which were further analysed using GISAXS. Characteristic parameters of the fluctuations such as average distance between neighbouring fluctuations, average size and lateral distribution of their position were obtained by fitting numerical simulations to the measured scattering images, and these parameters are in good agreement with the STEM observations. For the numerical simulations the density fluctuations were approximated as a set of spheroids distributed inside the Si layers as a 3D para­crystal (a lattice of spheroids with short-range ordering but lacking any long-range order). From GISAXS, the density of the material inside the density fluctuations is calculated to be 2.07 g cm−3 which is 89% of the bulk value of the deposited layer (2.33 g cm−3).
  • 机译 多层X射线分型术解决500 nm轴向分离
    摘要:Multi-slice X-ray ptychography offers an approach to achieve images with a nanometre-scale resolution from samples with thicknesses larger than the depth of field of the imaging system by modeling a thick sample as a set of thin slices and accounting for the wavefront propagation effects within the specimen. Here, we present an experimental demonstration that resolves two layers of nanostructures separated by 500 nm along the axial direction, with sub-10 nm and sub-20 nm resolutions on two layers, respectively. Fluorescence maps are simultaneously measured in the multi-modality imaging scheme to assist in decoupling the mixture of low-spatial-frequency features across different slices. The enhanced axial sectioning capability using correlative signals obtained from multi-modality measurements demonstrates the great potential of the multi-slice ptychography method for investigating specimens with extended dimensions in 3D with high resolution.
  • 机译 高速张量层析成像:迭代重建张量层析成像(IRTT)算法
    摘要:The recent advent of tensor tomography techniques has enabled tomographic investigations of the 3D nanostructure organization of biological and material science samples. These techniques extended the concept of conventional X-ray tomography by reconstructing not only a scalar value such as the attenuation coefficient per voxel, but also a set of parameters that capture the local anisotropy of nanostructures within every voxel of the sample. Tensor tomography data sets are intrinsically large as each pixel of a conventional X-ray projection is substituted by a scattering pattern, and projections have to be recorded at different sample angular orientations with several tilts of the rotation axis with respect to the X-ray propagation direction. Currently available reconstruction approaches for such large data sets are computationally expensive. Here, a novel, fast reconstruction algorithm, named iterative reconstruction tensor tomography (IRTT), is presented to simplify and accelerate tensor tomography reconstructions. IRTT is based on a second-rank tensor model to describe the anisotropy of the nanostructure in every voxel and on an iterative error backpropagation reconstruction algorithm to achieve high convergence speed. The feasibility and accuracy of IRTT are demonstrated by reconstructing the nanostructure anisotropy of three samples: a carbon fiber knot, a human bone trabecula specimen and a fixed mouse brain. Results and reconstruction speed were compared with those obtained by the small-angle scattering tensor tomography (SASTT) reconstruction method introduced by Liebi et al. [Nature (2015), 527, 349–352]. The principal orientation of the nanostructure within each voxel revealed a high level of agreement between the two methods. Yet, for identical data sets and computer hardware used, IRTT was shown to be more than an order of magnitude faster. IRTT was found to yield robust results, it does not require prior knowledge of the sample for initializing parameters, and can be used in cases where simple anisotropy metrics are sufficient, i.e. the tensor approximation adequately captures the level of anisotropy and the dominant orientation within a voxel. In addition, by greatly accelerating the reconstruction, IRTT is particularly suitable for handling large tomographic data sets of samples with internal structure or as a real-time analysis tool during the experiment for online feedback during data acquisition. Alternatively, the IRTT results might be used as an initial guess for models capturing a higher complexity of structural anisotropy such as spherical harmonics based SASTT in Liebi et al. (2015), improving both overall convergence speed and robustness of the reconstruction.
  • 机译 Y沸石中的CO2吸附:一种新颖的主成分分析辅助原位单晶X射线衍射实验的结构和动力学视图
    摘要:The increasing efficiency of detectors and brightness of X-rays in both laboratory and large-scale facilities allow the collection of full single-crystal X-ray data sets within minutes. The analysis of these ‘crystallographic big data’ requires new tools and approaches. To answer these needs, the use of principal component analysis (PCA) is proposed to improve the efficiency and speed of the analysis. Potentialities and limitations of PCA were investigated using single-crystal X-ray diffraction (XRD) data collected in situ on Y zeolite, in which CO2, acting as an active species, is thermally adsorbed while cooling from 300 to 200 K. For the first time, thanks to the high sensitivity of single-crystal XRD, it was possible to determine the sites where CO2 is adsorbed, the increase in their occupancy while the temperature is decreased, and the correlated motion of active species, i.e. CO2, H2O and Na+. PCA allowed identification and elimination of problematic data sets, and better understanding of the trends of the occupancies of CO2, Na+ and water. The quality of the data allowed for the first time calculation of the enthalpy (ΔH) and entropy (ΔS) of the CO2 adsorption by applying the van ’t Hoff equation to in situ single-crystal data. The calculation of thermodynamic values was carried out by both traditional and PCA-based approaches, producing comparable results. The obtained ΔH value is significant and involves systems (CO2 and Y zeolite) with no toxicity, superb stability and chemical inertness. Such features, coupled with the absence of carbonate formation and framework inertness upon adsorption, were demonstrated for the bulk crystal by the single-crystal experiment, and suggest that the phenomenon can be easily reversed for a large number of cycles, with CO2 released on demand. The main advantages of PCA-assisted analysis reside in its speed and in the possibility of it being applied directly to raw data, possibly as an ‘online’ data-quality test during data collection, without any a priori knowledge of the crystal structure.
  • 机译 SHELXL的非球面散射因子–模型,实施和应用
    摘要:A new aspherical scattering factor formalism has been implemented in the crystallographic least-squares refinement program SHELXL. The formalism relies on Gaussian functions and can optionally complement the independent atom model to take into account the deformation of electron-density distribution due to chemical bonding and lone pairs. Asphericity contributions were derived from the electron density obtained from quantum-chemical density functional theory computations of suitable model compounds that contain particular chemical environments, as defined by the invariom formalism. Thanks to a new algorithm, invariom assignment for refinement in SHELXL is automated. A suitable parameterization for each chemical environment within the new model was achieved by metaheuristics. Figures of merit, precision and accuracy of crystallographic least-squares refinements improve significantly upon using the new model.
  • 机译 二维富勒烯准晶体中的旋转开关
    • 作者:M. PaßensS. Karthäuser
    • 刊名:Acta Crystallographica. Section A, Foundations and Advances
    • 2019年第Pt 1期
    摘要:One of the essential components of molecular electronic circuits are switching elements that are stable in two different states and can ideally be switched on and off many times. Here, distinct buckminsterfullerenes within a self-assembled monolayer, forming a two-dimensional dodecagonal quasicrystal on a Pt-terminated Pt3Ti(111) surface, are identified to form well separated molecular rotational switching elements. Employing scanning tunneling microscopy, the molecular-orbital appearance of the fullerenes in the quasicrystalline monolayer is resolved. Thus, fullerenes adsorbed on the 36 vertex configuration are identified to exhibit a distinctly increased mobility. In addition, this finding is verified by differential conductance measurements. The rotation of these mobile fullerenes can be triggered frequently by applied voltage pulses, while keeping the neighboring molecules immobile. An extensive analysis reveals that crystallographic and energetic constraints at the molecule/metal interface induce an inequality of the local potentials for the 36 and 32.4.3.4 vertex sites and this accounts for the switching ability of fullerenes on the 36 vertex sites. Consequently, a local area of the 8/3 approximant in the two-dimensional fullerene quasicrystal consists of single rotational switching fullerenes embedded in a matrix of inert molecules. Furthermore, it is deduced that optimization of the intermolecular interactions between neighboring fullerenes hinders the realization of translational periodicity in the fullerene monolayer on the Pt-terminated Pt3Ti(111) surface.
  • 机译 出售还原与Niggli还原的晶格
    摘要:The unit-cell reduction described by Selling and used by Delone (whose early publications were under the spelling Delaunay) is explained in a simple form. The transformations needed to implement the reduction are listed. The simplicity of this reduction contrasts with the complexity of Niggli reduction.
  • 机译 利用混合流反应器对纳米级非晶态和晶体材料进行原位结构研究的新方法
    摘要:Structural investigations of amorphous and nanocrystalline phases forming in solution are historically challenging. Few methods are capable of in situ atomic structural analysis and rigorous control of the system. A mixed-flow reactor (MFR) is used for total X-ray scattering experiments to examine the short- and long-range structure of phases in situ with pair distribution function (PDF) analysis. The adaptable experimental setup enables data collection for a range of different system chemistries, initial supersaturations and residence times. The age of the sample during analysis is controlled by adjusting the flow rate. Faster rates allow for younger samples to be examined, but if flow is too fast not enough data are acquired to average out excess signal noise. Slower flow rates form older samples, but at very slow speeds particles settle and block flow, clogging the system. Proper background collection and subtraction is critical for data optimization. Overall, this MFR method is an ideal scheme for analyzing the in situ structures of phases that form during crystal growth in solution. As a proof of concept, high-resolution total X-ray scattering data of amorphous and crystalline calcium phosphates and amorphous calcium carbonate were collected for PDF analysis.
  • 机译 X射线衍射莫尔条纹特性的理论研究。一,勘误和补遗
    • 作者:Jun-ichi Yoshimura
    • 刊名:Acta Crystallographica. Section A, Foundations and Advances
    • 2019年第Pt 4期
    摘要:Seven corrections are made and several supplementary equations are added to the article by Yoshimura [].
  • 机译 实验获得和计算机模拟的硅晶体X射线非共面18光束针孔形貌仪
    摘要:Non-coplanar 18-beam X-ray pinhole topographs for a silicon crystal were computer simulated by fast Fourier transforming the X-ray rocking amplitudes that were obtained by solving the n-beam (n = 18) Ewald–Laue dynamical theory (E-L&FFT method). They were in good agreement with the experimentally obtained images captured using synchrotron X-rays. From this result and further consideration based on it, it has been clarified that the X-ray diffraction intensities when n X-ray waves are simultaneously strong in the crystal can be computed for any n by using the E-L&FFT method.
  • 机译 晶格表示和聚类的空间
    摘要:Algorithms for quantifying the differences between two lattices are used for Bravais lattice determination, database lookup for unit cells to select candidates for molecular replacement, and recently for clustering to group together images from serial crystallography. It is particularly desirable for the differences between lattices to be computed as a perturbation-stable metric, i.e. as distances that satisfy the triangle inequality, so that standard tree-based nearest-neighbor algorithms can be used, and for which small changes in the lattices involved produce small changes in the distances computed. A perturbation-stable metric space related to the reduction algorithm of Selling and to the Bravais lattice determination methods of Delone is described. Two ways of representing the space, as six-dimensional real vectors or equivalently as three-dimensional complex vectors, are presented and applications of these metrics are discussed. (Note: in his later publications, Boris Delaunay used the Russian version of his surname, Delone.)
  • 机译 1:3 A-位序钙钛矿形成的群理论分析
    • 作者:Mikhail V. Talanov
    • 刊名:Acta Crystallographica. Section A, Foundations and Advances
    • 2019年第Pt 2期
    摘要:The quadruple perovskites AA′3 B 4 X 12 are characterized by an extremely wide variety of intriguing physical properties, which makes them attractive candidates for various applications. Using group-theoretical analysis, possible 1:3 A-site-ordered low-symmetry phases have been found. They can be formed from a parent perovskite structure (archetype) as a result of real or hypothetical (virtual) phase transitions due to different structural mechanisms (orderings and displacements of atoms, tilts of octahedra). For each type of low-symmetry phase, the full set of order parameters (proper and improper order parameters), the calculated structure, including the space group, the primitive cell multiplication, splitting of the Wyckoff positions and the structural formula were determined. All ordered phases were classified according to the irreducible representations of the space group of the parent phase (archetype) and systematized according to the types of structural mechanisms responsible for their formation. Special attention is paid to the structural mechanisms of formation of the low-symmetry phase of the compounds known from experimental data, such as: CaCu3Ti4O12, CaCu3Ga2Sn2O12, CaMn3Mn4O12, Ce1/2Cu3Ti4O12, LaMn3Mn4O12, BiMn3Mn4O12 and others. For the first time, the phenomenon of variability in the choice of the proper order parameters, which allows one to obtain the same structure by different group-theoretical paths, is established. This phenomenon emphasizes the fundamental importance of considering the full set of order parameters in describing phase transitions. Possible transition paths from the archetype with space group to all 1:3 A-site-ordered perovskites are illustrated using the Bärnighausen tree formalism. These results may be used to identify new phases and interpret experimental results, determine the structural mechanisms responsible for the formation of low-symmetry phases as well as to understand the structural genesis of the perovskite-like phases. The obtained non-model group-theoretical results in combination with crystal chemical data and first-principles calculations may be a starting point for the design of new functional materials with a perovskite structure.
  • 机译 键合网络与团簇的稳定性:Al13TM4伪十倍曲面的案例研究
    摘要:Clusters, i.e. polyhedral geometric entities, are widely used to describe the structure of complex intermetallic compounds. However, little is generally known about their physical significance. The atomic and electronic structures of the Al13TM4 complex intermetallic compounds (TM = Fe, Co, Ru, Rh) have been investigated using a wide range of ab initio tools in order to examine the influence of the chemical composition on the pertinence of the bulk structure description based on 3D clusters. In addition, since surface studies were found to be a relevant approach to address the question of cluster stability in complex phases, the interplay of the cluster substructure with the 2D surface is addressed in the case of the Al13Co4(100) and Al13Fe4(010) surfaces.
  • 机译 用第一性原理计算表征调制结构:莫来石有序的统一超空间方案
    摘要:The benefit of computational methods applying density functional theory for the description and understanding of modulated crystal structures is investigated. A method is presented which allows one to establish, improve and test superspace models including displacive and occupational modulation functions from first-principles calculations on commensurate structures. The total energies of different configurations allow one to distinguish stable and less stable structure models. The study is based on a series of geometrically optimized superstructures of mullite (Al4+2xSi2−2xO10−x) derived from the superspace group Pbam(α0½)0ss. Despite the disordered and structurally complex nature of mullite, the calculations on ordered superstructures are very useful for determining the ideal Al/Si ordering in mullite, extracting atomic modulation functions as well as understanding the SiO2–Al2O3 phase diagram. The results are compared with experimentally established models which confirm the validity and utility of the presented method.
  • 机译 泰德·詹森(Ted Janssen)和非周期性晶体
    • 作者:Marc de Boissieu
    • 刊名:Acta Crystallographica. Section A, Foundations and Advances
    • 2019年第Pt 2期
    摘要:This article reviews some of Ted Janssen’s (1936–2017) major contributions to the field of aperiodic crystals. Aperiodic crystals are long-range ordered structures without 3D lattice translations and encompass incommensurately modulated phases, incommensurate composites and quasicrystals. Together with Pim de Wolff and Aloysio Janner, Ted Janssen invented the very elegant theory of superspace crystallography that, by adding a supplementary dimension to the usual 3D space, allows for a deeper understanding of the atomic structure of aperiodic crystals. He also made important contributions to the understanding of the stability and dynamics of aperiodic crystals, exploring their fascinating physical properties. He constantly interacted and collaborated with experimentalists, always ready to share and explain his detailed understanding of aperiodic crystals.

客服邮箱:kefu@zhangqiaokeyan.com

京公网安备:11010802029741号 ICP备案号:京ICP备15016152号-6 六维联合信息科技 (北京) 有限公司©版权所有
  • 客服微信

  • 服务号