Pub Date : 2024-07-31eCollection Date: 2024-08-01DOI: 10.1107/S1600576724004175
Wojciech A Sławiński, Christopher J Kerr, Yuanpeng Zhang, Helen Y Playford, Martin T Dove, Anthony E Phillips, Matthew G Tucker
This work introduces a completely rewritten version of the program RMCProfile (version 7), big-box, reverse Monte Carlo modelling software for analysis of total scattering data. The major new feature of RMCProfile7 is the ability to refine multiple phases simultaneously, which is relevant for many current research areas such as energy materials, catalysis and engineering. Other new features include improved support for molecular potentials and rigid-body refinements, as well as multiple different data sets. An empirical resolution correction and calculation of the pair distribution function as a back-Fourier transform are now also available. RMCProfile7 is freely available for download at https://rmcprofile.ornl.gov/.
{"title":"<i>RMCProfile7</i>: reverse Monte Carlo for multiphase systems.","authors":"Wojciech A Sławiński, Christopher J Kerr, Yuanpeng Zhang, Helen Y Playford, Martin T Dove, Anthony E Phillips, Matthew G Tucker","doi":"10.1107/S1600576724004175","DOIUrl":"10.1107/S1600576724004175","url":null,"abstract":"<p><p>This work introduces a completely rewritten version of the program <i>RMCProfile</i> (version 7), big-box, reverse Monte Carlo modelling software for analysis of total scattering data. The major new feature of <i>RMCProfile7</i> is the ability to refine multiple phases simultaneously, which is relevant for many current research areas such as energy materials, catalysis and engineering. Other new features include improved support for molecular potentials and rigid-body refinements, as well as multiple different data sets. An empirical resolution correction and calculation of the pair distribution function as a back-Fourier transform are now also available. <i>RMCProfile7</i> is freely available for download at https://rmcprofile.ornl.gov/.</p>","PeriodicalId":14950,"journal":{"name":"Journal of Applied Crystallography","volume":null,"pages":null},"PeriodicalIF":6.1,"publicationDate":"2024-07-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11299618/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141897500","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-07-29eCollection Date: 2024-08-01DOI: 10.1107/S1600576724005028
Krishna Prasad Khakurel, Gabriel Žoldák, Borislav Angelov, Jakob Andreasson
With the emergence of ultrafast X-ray sources, interest in following fast processes in small molecules and macromolecules has increased. Most of the current research into ultrafast structural dynamics of macromolecules uses X-ray free-electron lasers. In parallel, small-scale laboratory-based laser-driven ultrafast X-ray sources are emerging. Continuous development of these sources is underway, and as a result many exciting applications are being reported. However, because of their low flux, such sources are not commonly used to study the structural dynamics of macromolecules. This article examines the feasibility of time-resolved powder diffraction of macromolecular microcrystals using a laboratory-scale laser-driven ultrafast X-ray source.
随着超快 X 射线源的出现,人们对跟踪小分子和大分子中快速过程的兴趣与日俱增。目前对大分子超快结构动力学的研究大多使用 X 射线自由电子激光器。与此同时,基于实验室的小型激光驱动超快 X 射线源也在不断涌现。这些光源正在不断开发中,因此许多令人兴奋的应用也被报道出来。然而,由于其通量较低,这类光源并不常用于研究大分子结构动力学。本文探讨了使用实验室规模的激光驱动超快 X 射线源对大分子微晶体进行时间分辨粉末衍射的可行性。
{"title":"On the feasibility of time-resolved X-ray powder diffraction of macromolecules using laser-driven ultrafast X-ray sources.","authors":"Krishna Prasad Khakurel, Gabriel Žoldák, Borislav Angelov, Jakob Andreasson","doi":"10.1107/S1600576724005028","DOIUrl":"10.1107/S1600576724005028","url":null,"abstract":"<p><p>With the emergence of ultrafast X-ray sources, interest in following fast processes in small molecules and macromolecules has increased. Most of the current research into ultrafast structural dynamics of macromolecules uses X-ray free-electron lasers. In parallel, small-scale laboratory-based laser-driven ultrafast X-ray sources are emerging. Continuous development of these sources is underway, and as a result many exciting applications are being reported. However, because of their low flux, such sources are not commonly used to study the structural dynamics of macromolecules. This article examines the feasibility of time-resolved powder diffraction of macromolecular microcrystals using a laboratory-scale laser-driven ultrafast X-ray source.</p>","PeriodicalId":14950,"journal":{"name":"Journal of Applied Crystallography","volume":null,"pages":null},"PeriodicalIF":6.1,"publicationDate":"2024-07-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11299613/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141897473","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-07-29eCollection Date: 2024-08-01DOI: 10.1107/S1600576724005624
Martin A Karlsen, Jonas Billet, Songsheng Tao, Isabel Van Driessche, Simon J L Billinge, Dorthe B Ravnsbæk
Structural modelling of operando pair distribution function (PDF) data of complex functional materials can be highly challenging. To aid the understanding of complex operando PDF data, this article demonstrates a toolbox for PDF analysis. The tools include denoising using principal component analysis together with the structureMining, similarityMapping and nmfMapping apps available through the online service 'PDF in the cloud' (PDFitc, https://pdfitc.org/). The toolbox is used for both ex situ and operando PDF data for 3 nm TiO2-bronze nanocrystals, which function as the active electrode material in a Li-ion battery. The tools enable structural modelling of the ex situ and operando PDF data, revealing two pristine TiO2 phases (bronze and anatase) and two lithiated Li x TiO2 phases (lithiated versions of bronze and anatase), and the phase evolution during galvanostatic cycling is characterized.
对复杂功能材料的操作数对分布函数(PDF)数据进行结构建模极具挑战性。为了帮助理解复杂的操作数对分布函数数据,本文展示了一个 PDF 分析工具箱。工具包括利用主成分分析法进行去噪,以及通过在线服务 "云中的 PDF"(PDFitc,https://pdfitc.org/)提供的 structureMining、similarityMapping 和 nmfMapping 应用程序。该工具箱适用于 3 nm TiO2-青铜纳米晶体的原位和操作 PDF 数据,该晶体是锂离子电池的活性电极材料。该工具可对原位和运行状态下的 PDF 数据进行结构建模,揭示出两种原始 TiO2 相(青铜相和锐钛矿相)和两种锂化 Li x TiO2 相(青铜相和锐钛矿相的锂化版本),并对电静力循环过程中的相演化进行表征。
{"title":"<i>Operando</i> pair distribution function analysis of nanocrystalline functional materials: the case of TiO<sub>2</sub>-bronze nanocrystals in Li-ion battery electrodes.","authors":"Martin A Karlsen, Jonas Billet, Songsheng Tao, Isabel Van Driessche, Simon J L Billinge, Dorthe B Ravnsbæk","doi":"10.1107/S1600576724005624","DOIUrl":"10.1107/S1600576724005624","url":null,"abstract":"<p><p>Structural modelling of <i>operando</i> pair distribution function (PDF) data of complex functional materials can be highly challenging. To aid the understanding of complex <i>operando</i> PDF data, this article demonstrates a toolbox for PDF analysis. The tools include denoising using principal component analysis together with the <i>structureMining</i>, <i>similarityMapping</i> and <i>nmfMapping</i> apps available through the online service 'PDF in the cloud' (<i>PDFitc</i>, https://pdfitc.org/). The toolbox is used for both <i>ex situ</i> and <i>operando</i> PDF data for 3 nm TiO<sub>2</sub>-bronze nanocrystals, which function as the active electrode material in a Li-ion battery. The tools enable structural modelling of the <i>ex situ</i> and <i>operando</i> PDF data, revealing two pristine TiO<sub>2</sub> phases (bronze and anatase) and two lithiated Li <sub><i>x</i></sub> TiO<sub>2</sub> phases (lithiated versions of bronze and anatase), and the phase evolution during galvanostatic cycling is characterized.</p>","PeriodicalId":14950,"journal":{"name":"Journal of Applied Crystallography","volume":null,"pages":null},"PeriodicalIF":6.1,"publicationDate":"2024-07-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11299615/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141899351","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-07-17eCollection Date: 2024-08-01DOI: 10.1107/S160057672400517X
Weijian Zheng, Jun-Sang Park, Peter Kenesei, Ahsan Ali, Zhengchun Liu, Ian Foster, Nicholas Schwarz, Rajkumar Kettimuthu, Antonino Miceli, Hemant Sharma
High-energy X-ray diffraction methods can non-destructively map the 3D microstructure and associated attributes of metallic polycrystalline engineering materials in their bulk form. These methods are often combined with external stimuli such as thermo-mechanical loading to take snapshots of the evolving microstructure and attributes over time. However, the extreme data volumes and the high costs of traditional data acquisition and reduction approaches pose a barrier to quickly extracting actionable insights and improving the temporal resolution of these snapshots. This article presents a fully automated technique capable of rapidly detecting the onset of plasticity in high-energy X-ray microscopy data. The technique is computationally faster by at least 50 times than the traditional approaches and works for data sets that are up to nine times sparser than a full data set. This new technique leverages self-supervised image representation learning and clustering to transform massive data sets into compact, semantic-rich representations of visually salient characteristics (e.g. peak shapes). These characteristics can rapidly indicate anomalous events, such as changes in diffraction peak shapes. It is anticipated that this technique will provide just-in-time actionable information to drive smarter experiments that effectively deploy multi-modal X-ray diffraction methods spanning many decades of length scales.
高能 X 射线衍射方法可以非破坏性地绘制金属多晶工程材料的三维微观结构和相关属性。这些方法通常与热机械加载等外部刺激相结合,以拍摄随时间演变的微观结构和属性的快照。然而,传统的数据采集和还原方法数据量巨大、成本高昂,阻碍了快速提取可行见解和提高这些快照的时间分辨率。本文介绍了一种能够在高能 X 射线显微镜数据中快速检测可塑性开始的全自动技术。该技术的计算速度比传统方法至少快 50 倍,而且适用于比完整数据集稀疏 9 倍的数据集。这项新技术利用自监督图像表征学习和聚类,将海量数据集转化为紧凑、语义丰富的视觉显著特征(如峰值形状)表征。这些特征可迅速显示异常事件,如衍射峰形状的变化。预计这项技术将提供及时可操作的信息,以推动更智能的实验,有效部署跨越数十年长度尺度的多模态 X 射线衍射方法。
{"title":"Rapid detection of rare events from <i>in situ</i>X-ray diffraction data using machine learning.","authors":"Weijian Zheng, Jun-Sang Park, Peter Kenesei, Ahsan Ali, Zhengchun Liu, Ian Foster, Nicholas Schwarz, Rajkumar Kettimuthu, Antonino Miceli, Hemant Sharma","doi":"10.1107/S160057672400517X","DOIUrl":"10.1107/S160057672400517X","url":null,"abstract":"<p><p>High-energy X-ray diffraction methods can non-destructively map the 3D microstructure and associated attributes of metallic polycrystalline engineering materials in their bulk form. These methods are often combined with external stimuli such as thermo-mechanical loading to take snapshots of the evolving microstructure and attributes over time. However, the extreme data volumes and the high costs of traditional data acquisition and reduction approaches pose a barrier to quickly extracting actionable insights and improving the temporal resolution of these snapshots. This article presents a fully automated technique capable of rapidly detecting the onset of plasticity in high-energy X-ray microscopy data. The technique is computationally faster by at least 50 times than the traditional approaches and works for data sets that are up to nine times sparser than a full data set. This new technique leverages self-supervised image representation learning and clustering to transform massive data sets into compact, semantic-rich representations of visually salient characteristics (<i>e.g.</i> peak shapes). These characteristics can rapidly indicate anomalous events, such as changes in diffraction peak shapes. It is anticipated that this technique will provide just-in-time actionable information to drive smarter experiments that effectively deploy multi-modal X-ray diffraction methods spanning many decades of length scales.</p>","PeriodicalId":14950,"journal":{"name":"Journal of Applied Crystallography","volume":null,"pages":null},"PeriodicalIF":6.1,"publicationDate":"2024-07-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11299612/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141897477","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-07-11DOI: 10.1107/s1600576724004448
Tim T. Jäger, A. Losko, A. Wolfertz, Søren Schmidt, Mads Bertelsen, A. Khaplanov, Sean R. Agnew, F. Funama, Manuel Morgano, M. Roth, J. R. Gochanour, A. M. Long, Luca Lutterotti, S. Vogel
Neutron diffraction beamlines have traditionally relied on deploying large detector arrays of 3He tubes or neutron-sensitive scintillators coupled with photomultipliers to efficiently probe crystallographic and microstructure information of a given material. Given the large upfront cost of custom-made data acquisition systems and the recent scarcity of 3He, new diffraction beamlines or upgrades to existing ones demand innovative approaches. This paper introduces a novel Timepix3-based event-mode imaging neutron diffraction detector system as well as first results of a silicon powder diffraction measurement made at the HIPPO neutron powder diffractometer at the Los Alamos Neutron Science Center. Notably, these initial measurements were conducted simultaneously with the 3He array on HIPPO, enabling direct comparison. Data reduction for this type of data was implemented in the MAUD code, enabling Rietveld analysis. Results from the Timepix3-based setup and HIPPO were benchmarked against McStas simulations, showing good agreement for peak resolution. With further development, systems such as the one presented here may substantially reduce the cost of detector systems for new neutron instrumentation as well as for upgrades of existing beamlines.
{"title":"Demonstration of neutron time-of-flight diffraction with an event-mode imaging detector","authors":"Tim T. Jäger, A. Losko, A. Wolfertz, Søren Schmidt, Mads Bertelsen, A. Khaplanov, Sean R. Agnew, F. Funama, Manuel Morgano, M. Roth, J. R. Gochanour, A. M. Long, Luca Lutterotti, S. Vogel","doi":"10.1107/s1600576724004448","DOIUrl":"https://doi.org/10.1107/s1600576724004448","url":null,"abstract":"Neutron diffraction beamlines have traditionally relied on deploying large detector arrays of 3He tubes or neutron-sensitive scintillators coupled with photomultipliers to efficiently probe crystallographic and microstructure information of a given material. Given the large upfront cost of custom-made data acquisition systems and the recent scarcity of 3He, new diffraction beamlines or upgrades to existing ones demand innovative approaches. This paper introduces a novel Timepix3-based event-mode imaging neutron diffraction detector system as well as first results of a silicon powder diffraction measurement made at the HIPPO neutron powder diffractometer at the Los Alamos Neutron Science Center. Notably, these initial measurements were conducted simultaneously with the 3He array on HIPPO, enabling direct comparison. Data reduction for this type of data was implemented in the MAUD code, enabling Rietveld analysis. Results from the Timepix3-based setup and HIPPO were benchmarked against McStas simulations, showing good agreement for peak resolution. With further development, systems such as the one presented here may substantially reduce the cost of detector systems for new neutron instrumentation as well as for upgrades of existing beamlines.","PeriodicalId":14950,"journal":{"name":"Journal of Applied Crystallography","volume":null,"pages":null},"PeriodicalIF":6.1,"publicationDate":"2024-07-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141658873","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-07-11DOI: 10.1107/s1600576724004503
N. S. Murthy, David T. Grubb
Small-angle X-ray and neutron scattering (SAXS and SANS) patterns from certain semicrystalline polymers and liquid crystals contain discrete reflections from ordered assemblies and central diffuse scattering (CDS) from uncorrelated structures. Systems with imperfectly ordered lamellar structures aligned by stretching or by a magnetic field produce four distinct SAXS patterns: two-point `banana', four-point pattern, four-point `eyebrow' and four-point `butterfly'. The peak intensities of the reflections lie not on a layer line, or the arc of a circle, but on an elliptical trajectory. Modeling shows that randomly placed lamellar stacks modified by chain slip and stack rotation or interlamellar shear can create these forms. On deformation, the isotropic CDS becomes an equatorial streak with an oval, diamond or two-bladed propeller shape, which can be analyzed by separation into isotropic and oriented components. The streak has elliptical intensity contours, a natural consequence of the imperfect alignment of the elongated scattering objects. Both equatorial streaks and two- and four-point reflections can be fitted in elliptical coordinates with relatively few parameters. Equatorial streaks can be analyzed to obtain the size and orientation of voids, fibrils or surfaces. Analyses of the lamellar reflection yield lamellar spacing, stack orientation (interlamellar shear) angle α and chain slip angle ϕ, as well as the size distribution of the lamellar stacks. Currently available computational tools allow these microstructural parameters to be rapidly refined.
{"title":"Evolution of elliptical SAXS patterns in aligned systems","authors":"N. S. Murthy, David T. Grubb","doi":"10.1107/s1600576724004503","DOIUrl":"https://doi.org/10.1107/s1600576724004503","url":null,"abstract":"Small-angle X-ray and neutron scattering (SAXS and SANS) patterns from certain semicrystalline polymers and liquid crystals contain discrete reflections from ordered assemblies and central diffuse scattering (CDS) from uncorrelated structures. Systems with imperfectly ordered lamellar structures aligned by stretching or by a magnetic field produce four distinct SAXS patterns: two-point `banana', four-point pattern, four-point `eyebrow' and four-point `butterfly'. The peak intensities of the reflections lie not on a layer line, or the arc of a circle, but on an elliptical trajectory. Modeling shows that randomly placed lamellar stacks modified by chain slip and stack rotation or interlamellar shear can create these forms. On deformation, the isotropic CDS becomes an equatorial streak with an oval, diamond or two-bladed propeller shape, which can be analyzed by separation into isotropic and oriented components. The streak has elliptical intensity contours, a natural consequence of the imperfect alignment of the elongated scattering objects. Both equatorial streaks and two- and four-point reflections can be fitted in elliptical coordinates with relatively few parameters. Equatorial streaks can be analyzed to obtain the size and orientation of voids, fibrils or surfaces. Analyses of the lamellar reflection yield lamellar spacing, stack orientation (interlamellar shear) angle α and chain slip angle ϕ, as well as the size distribution of the lamellar stacks. Currently available computational tools allow these microstructural parameters to be rapidly refined.","PeriodicalId":14950,"journal":{"name":"Journal of Applied Crystallography","volume":null,"pages":null},"PeriodicalIF":6.1,"publicationDate":"2024-07-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141658021","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-07-04DOI: 10.1107/s1600576724004114
Mikhail Karnevskiy, K. Glazyrin, Yuelong Yu, Anshuman Mondal, Carmen Sanchez-Valle, Hauke Marquardt, R. Husband, Earl O'Bannon, C. Prescher, Anton Barty, H. Liermann
Presented and discussed here is the implementation of a software solution that provides prompt X-ray diffraction data analysis during fast dynamic compression experiments conducted within the dynamic diamond anvil cell technique. It includes efficient data collection, streaming of data and metadata to a high-performance cluster (HPC), fast azimuthal data integration on the cluster, and tools for controlling the data processing steps and visualizing the data using the DIOPTAS software package. This data processing pipeline is invaluable for a great number of studies. The potential of the pipeline is illustrated with two examples of data collected on ammonia–water mixtures and multiphase mineral assemblies under high pressure. The pipeline is designed to be generic in nature and could be readily adapted to provide rapid feedback for many other X-ray diffraction techniques, e.g. large-volume press studies, in situ stress/strain studies, phase transformation studies, chemical reactions studied with high-resolution diffraction etc.
本文介绍和讨论的软件解决方案可在动态金刚石砧室技术中进行的快速动态压缩实验期间提供及时的 X 射线衍射数据分析。它包括高效的数据收集、将数据和元数据流传输到高性能集群(HPC)、在集群上进行快速方位数据整合,以及使用 DIOPTAS 软件包控制数据处理步骤和可视化数据的工具。这一数据处理管道对大量研究都非常宝贵。以高压下的氨水混合物和多相矿物集合体的数据采集为例,说明了该管道的潜力。该管道的设计具有通用性,可随时调整,为许多其他 X 射线衍射技术提供快速反馈,例如大体积压制研究、原位应力/应变研究、相变研究、利用高分辨率衍射研究化学反应等。
{"title":"Automated pipeline processing X-ray diffraction data from dynamic compression experiments on the Extreme Conditions Beamline of PETRA III","authors":"Mikhail Karnevskiy, K. Glazyrin, Yuelong Yu, Anshuman Mondal, Carmen Sanchez-Valle, Hauke Marquardt, R. Husband, Earl O'Bannon, C. Prescher, Anton Barty, H. Liermann","doi":"10.1107/s1600576724004114","DOIUrl":"https://doi.org/10.1107/s1600576724004114","url":null,"abstract":"Presented and discussed here is the implementation of a software solution that provides prompt X-ray diffraction data analysis during fast dynamic compression experiments conducted within the dynamic diamond anvil cell technique. It includes efficient data collection, streaming of data and metadata to a high-performance cluster (HPC), fast azimuthal data integration on the cluster, and tools for controlling the data processing steps and visualizing the data using the DIOPTAS software package. This data processing pipeline is invaluable for a great number of studies. The potential of the pipeline is illustrated with two examples of data collected on ammonia–water mixtures and multiphase mineral assemblies under high pressure. The pipeline is designed to be generic in nature and could be readily adapted to provide rapid feedback for many other X-ray diffraction techniques, e.g. large-volume press studies, in situ stress/strain studies, phase transformation studies, chemical reactions studied with high-resolution diffraction etc.\u0000","PeriodicalId":14950,"journal":{"name":"Journal of Applied Crystallography","volume":null,"pages":null},"PeriodicalIF":6.1,"publicationDate":"2024-07-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141677444","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-07-04DOI: 10.1107/s1600576724004709
Natsuki Akaishi, Koki Yamada, Kohei Yatabe, Yuki Takayama
X-ray ptychography is a lensless imaging technique that visualizes the nanostructure of a thick specimen which cannot be observed with an electron microscope. It reconstructs a complex-valued refractive index of the specimen from observed diffraction patterns. This reconstruction problem is called phase retrieval (PR). For further improvement in the imaging capability, including expansion of the depth of field, various PR algorithms have been proposed. Since a high-quality PR method is built upon a base PR algorithm such as ePIE, developing a well performing base PR algorithm is important. This paper proposes an improved iterative algorithm named CRISP. It exploits subgradient projection which allows adaptive step size and can be expected to avoid yielding a poor image. The proposed algorithm was compared with ePIE, which is a simple and fast-convergence algorithm, and its modified algorithm, rPIE. The experiments confirmed that the proposed method improved the reconstruction performance for both simulation and real data.
X 射线层析成像技术是一种无透镜成像技术,可观察到电子显微镜无法观察到的厚试样的纳米结构。它根据观察到的衍射图样重建试样的复值折射率。这种重建问题被称为相位检索(PR)。为了进一步提高成像能力,包括扩大景深,人们提出了各种相位检索算法。由于高质量的相位检索方法建立在 ePIE 等基本相位检索算法的基础上,因此开发一种性能良好的基本相位检索算法非常重要。本文提出了一种名为 CRISP 的改进迭代算法。该算法利用子梯度投影,允许自适应步长,可望避免产生不良图像。本文将提出的算法与 ePIE(一种简单、收敛快的算法)及其改进算法 rPIE 进行了比较。实验证实,所提出的方法提高了模拟和真实数据的重建性能。
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Pub Date : 2024-07-04eCollection Date: 2024-08-01DOI: 10.1107/S1600576724004618
Anastasia Ragulskaya, Vladimir Starostin, Fajun Zhang, Christian Gutt, Frank Schreiber
X-ray photon correlation spectroscopy (XPCS) is a powerful tool for the investigation of dynamics covering a broad range of timescales and length scales. The two-time correlation function (TTC) is commonly used to track non-equilibrium dynamical evolution in XPCS measurements, with subsequent extraction of one-time correlations. While the theoretical foundation for the quantitative analysis of TTCs is primarily established for equilibrium systems, where key parameters such as the diffusion coefficient remain constant, non-equilibrium systems pose a unique challenge. In such systems, different projections ('cuts') of the TTC may lead to divergent results if the underlying fundamental parameters themselves are subject to temporal variations. This article explores widely used approaches for TTC calculations and common methods for extracting relevant information from correlation functions, particularly in the light of comparing dynamics in equilibrium and non-equilibrium systems.
X 射线光子相关光谱(XPCS)是研究涵盖广泛时间尺度和长度尺度的动力学的强大工具。在 XPCS 测量中,双时相关函数(TTC)通常用于跟踪非平衡动力学演化,并随后提取单时相关性。虽然定量分析 TTC 的理论基础主要是针对平衡系统建立的,在平衡系统中,扩散系数等关键参数保持不变,但非平衡系统带来了独特的挑战。在这类系统中,如果基本参数本身会发生时间变化,那么对 TTC 的不同预测("切割")可能会导致不同的结果。本文探讨了广泛使用的 TTC 计算方法,以及从相关函数中提取相关信息的常用方法,特别是在比较平衡和非平衡系统的动力学时。
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Pub Date : 2024-07-04eCollection Date: 2024-08-01DOI: 10.1107/S1600576724004527
Jaime Fernandez-Sanchez, Ana Cuesta, Shiva Shirani, Cinthya Redondo-Soto, Angeles G De la Torre, Isabel Santacruz, Ines R Salcedo, Laura Leon-Reina, Miguel A G Aranda
Portland cements (PCs) and cement blends are multiphase materials of different fineness, and quantitatively analysing their hydration pathways is very challenging. The dissolution (hydration) of the initial crystalline and amorphous phases must be determined, as well as the formation of labile (such as ettringite), reactive (such as portlandite) and amorphous (such as calcium silicate hydrate gel) components. The microstructural changes with hydration time must also be mapped out. To address this robustly and accurately, an innovative approach is being developed based on in situ measurements of pastes without any sample conditioning. Data are sequentially acquired by Mo Kα1 laboratory X-ray powder diffraction (LXRPD) and microtomography (µCT), where the same volume is scanned with time to reduce variability. Wide capillaries (2 mm in diameter) are key to avoid artefacts, e.g. self-desiccation, and to have excellent particle averaging. This methodology is tested in three cement paste samples: (i) a commercial PC 52.5 R, (ii) a blend of 80 wt% of this PC and 20 wt% quartz, to simulate an addition of supplementary cementitious materials, and (iii) a blend of 80 wt% PC and 20 wt% limestone, to simulate a limestone Portland cement. LXRPD data are acquired at 3 h and 1, 3, 7 and 28 days, and µCT data are collected at 12 h and 1, 3, 7 and 28 days. Later age data can also be easily acquired. In this methodology, the amounts of the crystalline phases are directly obtained from Rietveld analysis and the amorphous phase contents are obtained from mass-balance calculations. From the µCT study, and within the attained spatial resolution, three components (porosity, hydrated products and unhydrated cement particles) are determined. The analyses quantitatively demonstrate the filler effect of quartz and limestone in the hydration of alite and the calcium aluminate phases. Further hydration details are discussed.
硅酸盐水泥(PCs)和水泥混合料是不同细度的多相材料,对其水化途径进行定量分析非常具有挑战性。必须确定初始结晶相和无定形相的溶解(水化)情况,以及易溶组分(如埃特林特)、活性组分(如波长石)和无定形组分(如硅酸钙水合物凝胶)的形成情况。还必须绘制出微观结构随水化时间的变化图。为了稳健而准确地解决这一问题,我们正在开发一种创新方法,该方法基于对浆料的原位测量,无需对样品进行任何调节。通过 Mo Kα1 实验室 X 射线粉末衍射 (LXRPD) 和显微层析 (µCT) 顺序获取数据,在扫描过程中对同一体积进行扫描,以减少变化。宽毛细管(直径 2 毫米)是避免伪影(如自干燥)和获得优异颗粒平均性的关键。该方法在三种水泥浆样品中进行了测试:(i) 商品 PC 52.5 R,(ii) 80 wt% PC 和 20 wt% 石英的混合料,用于模拟添加胶凝补充材料,以及 (iii) 80 wt% PC 和 20 wt% 石灰石的混合料,用于模拟石灰石波特兰水泥。在 3 小时和 1、3、7 和 28 天时采集 LXRPD 数据,在 12 小时和 1、3、7 和 28 天时采集 µCT 数据。后期龄期数据也可轻松获取。在这种方法中,结晶相的数量可直接通过里特维尔德分析法获得,而非晶相的含量则可通过质量平衡计算获得。通过 µCT 研究,在达到的空间分辨率范围内,可以确定三种成分(孔隙率、水化产物和未水化水泥颗粒)。分析从数量上证明了石英和石灰石在水合铝土矿和铝酸钙相中的填充作用。还讨论了进一步的水化细节。
{"title":"Mix and measure II: joint high-energy laboratory powder diffraction and microtomography for cement hydration studies.","authors":"Jaime Fernandez-Sanchez, Ana Cuesta, Shiva Shirani, Cinthya Redondo-Soto, Angeles G De la Torre, Isabel Santacruz, Ines R Salcedo, Laura Leon-Reina, Miguel A G Aranda","doi":"10.1107/S1600576724004527","DOIUrl":"10.1107/S1600576724004527","url":null,"abstract":"<p><p>Portland cements (PCs) and cement blends are multiphase materials of different fineness, and quantitatively analysing their hydration pathways is very challenging. The dissolution (hydration) of the initial crystalline and amorphous phases must be determined, as well as the formation of labile (such as ettringite), reactive (such as portlandite) and amorphous (such as calcium silicate hydrate gel) components. The microstructural changes with hydration time must also be mapped out. To address this robustly and accurately, an innovative approach is being developed based on <i>in situ</i> measurements of pastes without any sample conditioning. Data are sequentially acquired by Mo <i>K</i>α<sub>1</sub> laboratory X-ray powder diffraction (LXRPD) and microtomography (µCT), where the same volume is scanned with time to reduce variability. Wide capillaries (2 mm in diameter) are key to avoid artefacts, <i>e.g.</i> self-desiccation, and to have excellent particle averaging. This methodology is tested in three cement paste samples: (i) a commercial PC 52.5 R, (ii) a blend of 80 wt% of this PC and 20 wt% quartz, to simulate an addition of supplementary cementitious materials, and (iii) a blend of 80 wt% PC and 20 wt% limestone, to simulate a limestone Portland cement. LXRPD data are acquired at 3 h and 1, 3, 7 and 28 days, and µCT data are collected at 12 h and 1, 3, 7 and 28 days. Later age data can also be easily acquired. In this methodology, the amounts of the crystalline phases are directly obtained from Rietveld analysis and the amorphous phase contents are obtained from mass-balance calculations. From the µCT study, and within the attained spatial resolution, three components (porosity, hydrated products and unhydrated cement particles) are determined. The analyses quantitatively demonstrate the filler effect of quartz and limestone in the hydration of alite and the calcium aluminate phases. Further hydration details are discussed.</p>","PeriodicalId":14950,"journal":{"name":"Journal of Applied Crystallography","volume":null,"pages":null},"PeriodicalIF":6.1,"publicationDate":"2024-07-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11299602/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141897471","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}