Journal of Applied Crystallography最新文献

{"title":"Prediction of the space group and cell volume by training a convolutional neural network with primitive 'ideal' diffraction profiles and its application to 'real' experimental data.","authors":"Hiroyuki Ozaki, Naoya Ishida, Tetsu Kiyobayashi","doi":"10.1107/S1600576725002419","DOIUrl":"10.1107/S1600576725002419","url":null,"abstract":"<p><p>This study describes a deep learning approach to predict the space group and unit-cell volume of inorganic crystals from their powder X-ray diffraction profiles. Using an inorganic crystallographic database, convolutional neural network (CNN) models were successfully constructed with the δ-function-like 'ideal' X-ray diffraction profiles derived solely from the intrinsic properties of the crystal structure, which are dependent on neither the incident X-ray wavelength nor the line shape of the profiles. We examined how the statistical metrics (<i>e.g.</i> the prediction accuracy, precision and recall) are influenced by the ensemble averaging technique and the multi-task learning approach; six CNN models were created from an identical data set for the former, and the space group classification was coupled with the unit-cell volume prediction in a CNN architecture for the latter. The CNN models trained in the 'ideal' world were tested with 'real' X-ray profiles for eleven materials such as TiO₂, LiNiO₂ and LiMnO₂. While the models mostly fared well in the 'real' world, the cases at odds were scrutinized to elucidate the causes of the mismatch. Specifically for Li₂MnO₃, detailed crystallographic considerations revealed that the mismatch can stem from the state of the specific material and/or from the quality of the experimental data, and not from the CNN models. The present study demonstrates that we can obviate the need for emulating experimental diffraction profiles in training CNN models to elicit structural information, thereby focusing efforts on further improvements.</p>","PeriodicalId":14950,"journal":{"name":"Journal of Applied Crystallography","volume":"58 Pt 3","pages":"718-730"},"PeriodicalIF":6.1,"publicationDate":"2025-04-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12135985/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144234179","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}

{"title":"Rheo-SAXS study on electrically responsive hydro-gels with shear-induced conductive micellar networks for on-demand drug release.","authors":"Thuy Thien Ngan Vo, Yi-Wei Chang, Chun-Jen Su, U-Ser Jeng, Chih-Chia Cheng, Ya-Sen Sun, Wei-Tsung Chuang","doi":"10.1107/S1600576725002808","DOIUrl":"10.1107/S1600576725002808","url":null,"abstract":"<p><p>This study presents a novel approach to creating electrically responsive hydro-gels utilizing a poly(ethyl-ene oxide)-poly(propyl-ene oxide)-poly(ethyl-ene oxide) (PEO₁₀₀-PPO₆₅-PEO₁₀₀) triblock copolymer, functionalized with benzene-sulfonate end groups to form sF127. This functionalization allows the incorporation of sF127 into F127 micelles, resulting in tailored micelles designated as F₁₈S₂P when combined with poly(3,4-ethyl-ene-dioxy-thio-phene):poly(benzene-sulfonate) (PEDOT:PSS). For comparison, a control system using non-functionalized PEDOT:PSS/F127 micelles, designated F₂₀S₀P, was also developed. Using piroxicam as a model hydro-phobic drug, we evaluated the hydro-gel's drug encapsulation efficiency and electrical responsiveness. The functionalized F₁₈S₂P hydro-gel demonstrated superior performance of electrically stimulated drug release, especially when prepared with a blade-coating process. <i>In situ</i> rheological small-angle X-ray scattering (rheo-SAXS) measurements under large amplitude oscillatory shear revealed that function-alization facilitates crystal plane sliding, leading to the formation of a randomly hexagonal close-packed (rHCP) sliding layer structure. This behavior contrasts with the face-centered cubic to rHCP phase transition observed in the unfunctionalized hydro-gel. <i>In situ</i> SAXS analysis under applied electric fields (E-SAXS) further confirmed the electroresponsive micellar deformation. By integrating the rheo-SAXS and E-SAXS findings with blade-coating processing insights, we identify a clear structure-function relationship that governs the performance of these hydro-gels. The enhanced drug delivery of the function-al-ized F₁₈S₂P hydro-gel is attributed to the electrostatic attraction between the positively charged PEDOT and the negatively charged benzene-sulfonate-functionalized micelles. This interaction creates conductive nanonetworks within the hydro-gel, significantly improving its ability to release drugs in response to electrical stimulation. This work highlights the potential of electrically responsive hydro-gels for precise, localized drug delivery applications.</p>","PeriodicalId":14950,"journal":{"name":"Journal of Applied Crystallography","volume":"58 Pt 3","pages":"909-918"},"PeriodicalIF":6.1,"publicationDate":"2025-04-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12135972/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144234180","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}

{"title":"New features in <i>ATSAS-4</i>, a program suite for small-angle scattering data analysis.","authors":"D Franke, T Gräwert, D I Svergun","doi":"10.1107/S1600576725002481","DOIUrl":"10.1107/S1600576725002481","url":null,"abstract":"<p><p>The <i>ATSAS</i> release 4 series introduces substantial architectural updates and enhanced user-friendly tools for analyzing biological macromolecules and nanostructured objects. In particular, highly requested project support for graphical user interfaces (GUIs) has been implemented. Here the state of the main window of each GUI application can be saved as a project and then restored to continue or extend analyses. All GUI applications now share a common framework, enabling various plot annotations and export as figures or text for easy data exchange with other plotting applications. The main interactive data processing and interpretation program, <i>PRIMUS</i>, has been significantly expanded with new features and integrated analysis modules. A new GUI for the program <i>PEAK</i> allows for multiple fitting functions, including Gaussian, Lorentzian and pseudo-Voigt. The online chromatography analysis program <i>CHROMIXS</i> supports multiple frame selections and subtractions, along with a newly included <i>EFAMIX</i> module for resolving partially overlapping components. The new <i>ATSAS</i> application <i>LAUNCHER</i> provides user-friendly wizards to configure and run command-line applications. Wherever feasible, operations like file reading and calculations have been parallelized to take advantage of available local compute resources. Command-line interfaces of many applications have been updated, <i>e.g.</i> with renaming and unification of common options. Improved readers/writers are implemented for Protein Data Bank and macromolecular CIF (mmCIF) file handling. The program <i>MIXTURES</i> now combines the functionalities of <i>BILMIX</i>, <i>LIPMIX</i> and <i>MIXTURE</i>, offering simplified and more versatile analyses for polydisperse systems of different shapes, also with single- or multi-layered organization. Installer packages of <i>ATSAS</i> are available for the latest versions of Windows, frequently used Linux distributions and recent macOS releases, both for Intel and ARM architectures, and are free for academic use.</p>","PeriodicalId":14950,"journal":{"name":"Journal of Applied Crystallography","volume":"58 Pt 3","pages":"1027-1033"},"PeriodicalIF":6.1,"publicationDate":"2025-04-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12135997/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144234176","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}

{"title":"Structure factors of random hard disk packing in 2D by explicit modeling.","authors":"Yoshiharu Nishiyama","doi":"10.1107/S1600576725002407","DOIUrl":"10.1107/S1600576725002407","url":null,"abstract":"<p><p>This paper describes a method that can (1) generate random packing of hard disks in 2D using Monte Carlo simulation, (2) extract the corresponding pair distribution function using normalization by disk line picking probability and (3) convert it to the structure factor. The generated structure factor agrees well with the analytical form based on the Percus-Yevick equation at a low area fraction (that is, within 1% at an area fraction below 0.2 and 2% at an area fraction of 0.3) but differs at a higher area fraction with more pronounced peaks and oscillations. Above an area fraction of 0.69, the hexagonal packing feature appears as sharp peaks at low <i>Q</i>, which are absent in the analytical solution. The structure factors up to an area fraction of 0.65 as a function of <i>QR</i> and the area fraction are stored in table form. The structure factor table can be combined with the cylinder form factors to simulate the X-ray/neutron scattering intensity of wood cell wall scattering.</p>","PeriodicalId":14950,"journal":{"name":"Journal of Applied Crystallography","volume":"58 Pt 3","pages":"1015-1021"},"PeriodicalIF":6.1,"publicationDate":"2025-04-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12135971/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144234184","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}

{"title":"Local orthorhombic phase in zirconium oxide nanocrystals: insights from X-ray pair distribution function analysis.","authors":"Rohan Pokratath, Kumara Cordero-Edwards, Maryame Bina, Simon J L Billinge, Jonathan De Roo","doi":"10.1107/S1600576725001761","DOIUrl":"10.1107/S1600576725001761","url":null,"abstract":"<p><p>Zirconium dioxide (ZrO₂) and hafnium dioxide (HfO₂) have emerged as promising alternatives to conventional ferroelectric materials. Understanding the crystal phases of these oxides under different conditions is crucial for optimizing their properties. There are several theories for the (anti)ferroelectric properties; however, comprehensive analysis, particularly at the local structure level, is lacking. In this study, we investigate the local structure of ZrO₂ nanocrystals using X-ray pair distribution function (PDF) analysis, revealing an unexpected local orthorhombic distortion irrespective of crystallite size. This finding suggests the potential existence of an intermediate orthorhombic phase during the microscopic switching pathway observed in previous studies. Additionally, we explore the influence of crystallite size and surface effects on the PDF. These results contribute to a deeper understanding of the structural dynamics in ZrO₂ and offer insights for the design of next-generation ferroelectric materials.</p>","PeriodicalId":14950,"journal":{"name":"Journal of Applied Crystallography","volume":"58 Pt 3","pages":"688-695"},"PeriodicalIF":6.1,"publicationDate":"2025-04-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12135986/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144234174","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}

{"title":"Strain-induced density fluctuations in linear low-density polyethyl-ene.","authors":"Mizuki Kishimoto, Kazuki Mita, Hiroki Ogawa, Kazuki Shibasaki, Masato Arakawa, Mikihito Takenaka","doi":"10.1107/S1600576725002183","DOIUrl":"10.1107/S1600576725002183","url":null,"abstract":"<p><p>In our previous study [Kishimoto <i>et al.</i> (2020). <i>Macromolecules</i>, <b>53</b>, 9097-9107], density fluctuations were induced on the submicrometre scale in polyethyl-ene (PE) during strain and led to the generation of voids. The strength of the induction was found to increase with the amplitude of the spatial inhomogeneity of the stress field. In this work, we investigated how comonomer species and content affect the behaviors of the strain-induced density fluctuations in linear low-density PE. We found that the strength of the induction decreased with an increase in the spatial homogeneity before stretching and the mechanical melting during strain and that the degree of spatial homogeneity and mechanical melting depend on the species and content of the comonomer.</p>","PeriodicalId":14950,"journal":{"name":"Journal of Applied Crystallography","volume":"58 Pt 3","pages":"879-885"},"PeriodicalIF":6.1,"publicationDate":"2025-04-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12135982/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144234183","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}

{"title":"Synthesis and quantum crystallographic evaluation of WYLID: YLID's red rival.","authors":"Florian Meurer, Maximilian Schimpf, Birgit Hischa, Christoph Hennig, Julia Rehbein, Florian Kleemiss, Michael Bodensteiner","doi":"10.1107/S160057672500175X","DOIUrl":"10.1107/S160057672500175X","url":null,"abstract":"<p><p>The synthesis and characterization of WYLID [2-(di-methyl-λ⁴-sulfane-ylidene)-[1,2'-bi-indenyl-idene]-1',3,3'(2<i>H</i>)-trione], a side product that appears during the synthesis of YLID, is presented in this study. Quantum crystallographic insights into the bonding situation in WYLID are provided on the basis of Hirshfeld atom refinement (HAR), multipolar modelling and X-ray restrained wavefunction fitting. We compare these results with theoretical calculations on a gas-phase optimized density functional theory and a Hartree-Fock calculation based on the geometry obtained by HAR. The S-C bond in WYLID is best described as an ylid-type bond and the SMe₂ fragment does not affect the nearest C-O carbonyl/enolate equilibrium. This work may contribute to an ongoing debate in the quantum crystallography community about the bonding situation in YLID and provides a routine for distinguishing between carbonyls and enolates.</p>","PeriodicalId":14950,"journal":{"name":"Journal of Applied Crystallography","volume":"58 Pt 3","pages":"678-687"},"PeriodicalIF":6.1,"publicationDate":"2025-04-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12135977/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144234185","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}

{"title":"Reliability of pair distribution function analysis in <i>in situ</i> experiments.","authors":"Rasmus Baden Stubkjær, Magnus Kløve, Andreas Bertelsen, Anders Bæk Borup, Martin Roelsgaard, Bo Brummerstedt Iversen","doi":"10.1107/S1600576725001694","DOIUrl":"10.1107/S1600576725001694","url":null,"abstract":"<p><p><i>In situ</i> and <i>operando</i> pair distribution function (PDF) studies are becoming commonly used to study chemical reactions, nucleation and growth of nanoparticles, or structural changes during the operation of batteries, catalysts, thermoelectric devices <i>etc.</i> However, repeated time-resolved total scattering experiments and subsequent PDF analysis are often not prioritized due to the scarce synchrotron beam time available. This means that the experimental uncertainty and reproducibility of the experimental methods are unknown, and the full potential of <i>in situ</i> PDF experiments may not be exploited. Here, we quantify the experimental uncertainty of the PDF technique in an <i>in situ</i> study of the hydro-thermal synthesis of ZrO₂ nanoparticles. Systematic variation of the parameters used to obtain the PDF shows that the user-defined parameters can potentially affect the chemical conclusions obtained from the time-resolved experiment. We found that comparable results are best obtained using the same input parameters across different experiments. We also compare different PDF algorithms to examine whether the processing algorithm influences the chemical analysis.</p>","PeriodicalId":14950,"journal":{"name":"Journal of Applied Crystallography","volume":"58 Pt 2","pages":"495-503"},"PeriodicalIF":6.1,"publicationDate":"2025-03-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11957418/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143763416","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}

{"title":"Upgrade of the KWS-2 high-intensity/extended-<i>Q</i>-range SANS diffractometer of JCNS for soft matter and biophysics: <i>in situ</i> SEC, controlled <i>in situ</i> RH/T variation and WANS detection.","authors":"Jia-Jhen Kang, Ralf Biehl, Georg Brandl, Helmut Korb, Kimio Yoshimura, Vladimir Ossovyi, Andreas Nebel, Jacqueline Lippertz, Ralf Engels, Günter Kemmerling, Alexander Zaft, Hiroki Iwase, Hiroshi Arima-Osonoi, Shin-Ichi Takata, Alexander Weber, Simon Staringer, Baohu Wu, Yue Zhao, Stefan Mattauch, Aurel Radulescu","doi":"10.1107/S160057672500158X","DOIUrl":"10.1107/S160057672500158X","url":null,"abstract":"<p><p>The KWS-2 small-angle neutron scattering (SANS) diffractometer operated by Jülich Centre for Neutron Science (JCNS) at Heinz Maier-Leibnitz Zentrum, Garching, Germany, is dedicated to the investigation of mesoscopic multi-scale structures and structural changes due to rapid kinetic processes in soft condensed matter and biophysical systems. Following requests from the user community, it has been repeatedly upgraded with respect to the most important methodological parameters of an instrument of this type, namely the intensity on the sample, the instrumental resolution and the minimum scattering variable <i>Q</i> _min. Here we report on further specific improvements to the sample environment and detection capabilities which have just been completed or are being implemented. Complementary size-exclusion chromatography (SEC) for <i>in situ</i> protein purification was developed and optimized at KWS-2 to provide the instrument with biological samples of controlled quality. The instrument is also currently being equipped with a wide-angle neutron scattering (WANS) detector which will allow it to bridge the atomic and mesoscale, benefiting from the instrument's adjustable resolution down to Δλ/λ = 2%. For controlled relative humidity and temperature (RH/T) on ionic conductive samples for energy applications or biomembranes for biophysical and health applications, a precise dew point generator has recently been characterized and commissioned; this offers great versatility with regard to varying the contrast <i>in situ</i> in the beam on hydrated samples.</p>","PeriodicalId":14950,"journal":{"name":"Journal of Applied Crystallography","volume":"58 Pt 2","pages":"581-594"},"PeriodicalIF":6.1,"publicationDate":"2025-03-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11957400/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143763624","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}

{"title":"Solvent-annealing-induced microphase separation in polyether polyurethane: a small-angle X-ray scattering study.","authors":"Shanshan Wang, Jiayao Song, Keping Chen, Mark Julian Henderson, Qiang Tian, László Almásy","doi":"10.1107/S1600576725001633","DOIUrl":"10.1107/S1600576725001633","url":null,"abstract":"<p><p>This study investigated the effects of solvent vapor annealing on the microphase separation structure of polyurethane (PU) using small-angle X-ray scattering (SAXS) and complementary techniques. Solvent annealing, as an alternative to thermal annealing, offers a lower-temperature method to refine the microstructure of PU. We examined the impact of methyl ethyl ketone (MEK), acetone and toluene vapors on a commercial polyether PU, focusing on changes in microphase structure, adsorption kinetics and thermal stability. The SAXS data, analyzed by a polydisperse hard-sphere model, indicated that the degree of phase separation increased upon solvent annealing, and the order of influence exerted by the solvent vapors on the microphase structure follows MEK > acetone > toluene. The <i>in situ</i> variable-temperature SAXS results showed that the solvent-annealed sample had superior thermal stability to the quenched sample. Compared with high-temperature annealing, solvent annealing induced a higher degree of phase separation but did not lead to significant growth of the hard-urethane-segment-rich domains. These findings provide valuable insights into optimizing solvent annealing processes, allowing for advanced applications of PUs where excessive heat may lead to degradation or other undesirable changes.</p>","PeriodicalId":14950,"journal":{"name":"Journal of Applied Crystallography","volume":"58 Pt 2","pages":"564-572"},"PeriodicalIF":6.1,"publicationDate":"2025-03-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11957403/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143763635","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}