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Creation of crystal structure reproducing X-ray diffraction pattern without using database
发布时间:2023-09-19

Creation of crystal structure reproducing X-ray diffraction pattern without using database

   Joohwi Lee, Junpei Oba, Nobuko Ohba & Seiji Kajita  
 

    npj Computational Materials 9: 135 (2023)
   doi.org/10.1038/s41524-023-01096-3
    Published online: 05 August 2023
   AbstractFull Text | PDF OPEN
  

  
Abstract: When a sample’s X-ray diffraction pattern (XRD) is measured, the corresponding crystal structure is usually determined by searching for similar XRD patterns in the database. However, if a similar XRD pattern is not found, it is tremendously laborious to identify the crystal structure even for experts. This case commonly happens when researchers develop novel and complex materials. In this study, we propose a crystal structure creation scheme that reproduces a given XRD pattern. We employed a combinatorial inverse design method using an evolutionary algorithm and crystal morphing (Evolv&Morph) supported by Bayesian optimization, which maximizes the similarity of the XRD patterns between target one and those of the created crystal structures. For sixteen different crystal structure systems with twelve simulated and four powder target XRD patterns, Evolv&Morph successfully created crystal structures with the same XRD pattern as the target (cosine similarity 99% for the simulated ones and >96% the experimentally measured ones). Furthermore, the present method has merits in that it is an automated crystal structure creation scheme, not dependent on a database. We believe that Evolv&Morph can be applied not only to determine crystal structures but also to design materials for specific properties.
摘要:  半导体纳米晶体(NC)基器件的效率受非辐射过程的影响。其中一个关键过程是热激子冷却,即高度激发的电子-空穴对的非辐射弛豫,以形成带边激子。由于量子限域效应,冷却的时间尺度和机制尚不完全清楚。电子能隙与声子频率之间的不匹配导致了声子瓶颈和极其缓慢冷却的假设,而增强的电子-空穴相互作用则暗示了超快冷却。对冷却时间尺度的实验测量范围涵盖了六个数量级。在这里,我们采用原子尺度的方法来描述声子介导的激子动力学,并模拟在实验相关尺寸的NC中的冷却过程。我们发现,在CdSe半导体纳米晶体中,冷却发生在约30飞秒的时间尺度上,与最近的测量结果一致,并且通过多声子介导的级联弛豫事件,规避了声子瓶颈。此外,我们还确定了调节冷却时间尺度的NC参数。
Editorial Summary

Automated reverse design: Crystal structure reduction

Synthesizing ideal crystal structures is crucial for materials research, and X-ray diffraction (XRD) analysis has become the primary means to reveal their atomic and molecular structures by determining crystal phases, orientations, lattice parameters and grain sizes. With the support of material databases, XRD analysis is supported by large databases such as ICDD? and ICSD in order to simulate XRD patterns to determine the crystal structure, but conventional methods are limited when faced with XRD patterns of unknown structure. Methods such as machine learning, prototype search and deep learning have emerged in recent years to work towards more accurate and efficient crystal structure identification, while techniques such as Rietveld refinement can correct XRD patterns, and the recently proposed BBO-Rietveld method automatically adjusts the parameters to improve the success rate. However, Rietveld refinement relying on the initial structure is still imperfect, so there is an urgent need for an inverse design method that can directly generate the crystal structure of the target XRD pattern without database support. A team lead by Dr. Joohwi Lee from Toyota Central R&D Labs., Japan, proposed an automated crystal structure creation method, consisting of the evolutionary algorithm and crystal morphing supported by Bayesian optimization (Evolv&Morph), for reproducing the XRD pattern. The method optimizes the similarity score of XRD patterns of the created structures and the target. The evolutionary algorithm can automatically create various structures by genetic operators without input structures. Crystal morphing, using the input structures obtained by the evolutionary algorithm, expands search space and further increases the similarity of XRD patterns creating a better input structure for the post-refinement. After the refinement, for twelve binary and ternary systems in different crystal structures where the target XRD patterns were provided by simulation from the measured structures, Evolv&Morph achieves cosine similarity of ~99%. In addition, for four different powder XRD patterns, the present method achieved cosine similarity of of ~96%, after removal of background. These results indicate that the created crystal structure successfully reproduces the target XRD pattern. Therefore, the present method can identify unknown crystal structures after getting XRD measurement without depending on DB. Furthermore, Evolv&Morph can play a role of inverse design, which indicates that the desired property is defined first and the materials with such property are automatically searched. The optimization target score, which corresponds to the cosine similarity of the XRD pattern used in this study, can be exchanged for particular functional property according to the goal of the material design; therefore, the present method has a powerful potential to be applicable to material design, as well as crystal structure determination.
自动逆向设计:利用Evolv&Morph实现目标XRD图谱的晶体结构还原

合成理想晶体结构对材料研究至关重要,而X射线衍射(XRD)分析成为揭示其原子及分子结构的主要手段,可测定晶体相、取向、晶格参数和晶粒尺寸。在材料数据库的支持下,XRD分析借助大型数据库如ICDD?和ICSD,以模拟XRD图谱来确定晶体结构,但面对未知结构的XRD图谱时,传统方法有限。近年涌现的方法,如机器学习、原型搜索和深度学习,致力于更准确有效的晶体结构识别,而Rietveld细化等技术则可校正XRD图谱,最近提出的BBO-Rietveld方法能自动调整参数以提高成功率。然而,依赖初始结构的Rietveld改进仍不完美,因此急需一种逆设计方法,可在无需数据库支持下,直接生成目标XRD图谱的晶体结构。来自日本丰田中央研发实验室的Joohwi Lee博士领导的团队,提出了一种自动生成晶体结构的方法,该方法整合了进化算法和贝叶斯优化,以支持晶体变形(Evolv&Morph)技术,用于生成与目标XRD图谱相匹配的晶体结构。该方法中,进化算法能够自动产生多样的结构,无需外部输入。晶体变形利用进化算法得到的输入结构,扩大了搜索空间,进一步提高了XRD图谱的相似性,为后期细化创造了更好的输入结构。在细化阶段,针对12种不同的二元和三元体系,通过模拟测量结构得到目标XRD图谱,Evolv&Morph取得了约99%的余弦相似度。此外,对于四种不同的粉末XRD图谱,去除背景后,该方法的余弦相似度达到了~96%。这些结果明确表明,通过该方法成功地再现了目标XRD图谱的晶体结构。因此,该方法具备识别未知晶体结构的能力,而且无需依赖于外部数据库。此外,Evolv&Morph还能够进行逆向设计,即首先定义所需属性,然后自动搜索具备这些属性的材料。优化目标分数对应于本研究中使用的XRD图谱的余弦相似度,可以根据材料设计的目标,获取特定的功能性质;因此,这种方法在材料设计和晶体结构测定方面具有巨大的应用潜力。

 
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