利用中子全散射数据完善整个纳米粒子的方法和挑战

IF 5.2 3区 材料科学 Q2 CHEMISTRY, MULTIDISCIPLINARY
Bernadette Cladek, Yuanpeng Zhang, Russell Maier, Bruce Ravel, Matthew G. Tucker, Igor Levin
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引用次数: 0

摘要

本研究考虑了从飞行时间中子全散射明确确定纳米粒子中原子排列所需的关键数据还原步骤和数据分析方法。文中介绍了一种实用程序,用于去除大多数纳米粒子样品中不可避免存在的氢的非相干散射引起的寄生背景,并将恢复的相干散射强度归一化为绝对尺度。报告还介绍了对从总散射中得出的对分布函数的无模型分析,该分析可用于在不了解材料结构的情况下直接从实验数据中确定热膨胀系数和粒子尺寸。最后,使用 RMCProfile 软件中实施的反向蒙特卡罗方法,演示了根据中子全散射数据对掺钇铈纳米粒子进行原子全纳米细化。这些结果揭示了阳氧距离和氧氧距离对配位数的强烈依赖性,这导致了这些距离在颗粒表面附近的梯度。具体情况取决于配体和吸附剂的表面覆盖率以及纳米晶体团聚体的晶界结构。改进后的模型证实了粒子表面存在更严重的无序,扭曲的表面层延伸到多个配位层的预期。这些结果突显了根据中子数据对整个纳米粒子进行细化的可行性,要求进一步开发数据还原和分析程序。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Approaches and challenges in whole-nanoparticle refinements from neutron total-scattering data

Approaches and challenges in whole-nanoparticle refinements from neutron total-scattering data

This study considers critical data reduction steps and data analysis approaches required to determine explicitly the atomic arrangements in nanoparticles from time-of-flight neutron total scattering. A practical procedure is described for removing parasitic backgrounds caused by the incoherent scattering of hydrogen inevitably present in most nanoparticle samples and normalizing the recovered coherent scattering intensities onto an absolute scale. A model-free analysis is presented of a pair-distribution function derived from total scattering that can be used to determine thermal expansion coefficients and particle sizes directly from experimental data without knowledge of the material's structure. Finally, atomistic whole-nanoparticle refinements of yttrium-doped ceria nanoparticles from neutron total-scattering data are demonstrated using the reverse Monte Carlo method implemented in the RMCProfile software. These results reveal a strong dependence of the cation–oxygen and oxygen–oxygen distances on the coordination numbers, which leads to gradients of these distances near the particle surface. The details are dependent on the surface coverage by ligands and adsorbates and on the structure of grain boundaries in nanocrystalline agglomerates. The refined models confirm the expectations of more substantial disorder at particle surfaces, with a distorted surface layer extending over several coordination shells. The results highlight the feasibility of whole-nanoparticle refinements from neutron data, calling for further development of data reduction and analysis procedures.

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来源期刊
Journal of Applied Crystallography
Journal of Applied Crystallography CHEMISTRY, MULTIDISCIPLINARYCRYSTALLOGRAPH-CRYSTALLOGRAPHY
CiteScore
7.80
自引率
3.30%
发文量
178
期刊介绍: Many research topics in condensed matter research, materials science and the life sciences make use of crystallographic methods to study crystalline and non-crystalline matter with neutrons, X-rays and electrons. Articles published in the Journal of Applied Crystallography focus on these methods and their use in identifying structural and diffusion-controlled phase transformations, structure-property relationships, structural changes of defects, interfaces and surfaces, etc. Developments of instrumentation and crystallographic apparatus, theory and interpretation, numerical analysis and other related subjects are also covered. The journal is the primary place where crystallographic computer program information is published.
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