Review
Chemistry, Multidisciplinary
Maxwell W. Terban, Simon J. L. Billinge
Summary: This article reviews the application of atomic pair distribution function (PDF) analysis in the study of molecular materials. The PDF method is a powerful tool for investigating short- and intermediate-range order in nanoscale materials. It can provide structural details that are obscured in reciprocal space by defects, disorder, or structural ambiguities. While its use in inorganic and nanomaterials research has been highlighted, significant progress has also been made in applying PDF analysis to molecular materials such as carbon, pharmaceuticals, polymers, liquids, coordination compounds, and composites. The article provides an overview of applications in a wide variety of molecular compounds and systems, and offers pedagogical descriptions and tips for implementation.
Review
Chemistry, Multidisciplinary
Nora K. Zimmerli, Christoph R. Mueller, Paula M. Abdala
Summary: Heterogeneous catalysts are complex materials that require advanced structural characterization tools to determine structure-performance relationships. Pair distribution function (PDF) analysis is a powerful method for extracting structural information from the atomic to the nanoscale.
TRENDS IN CHEMISTRY
(2022)
Review
Chemistry, Multidisciplinary
He Zhu, Yalan Huang, Jincan Ren, Binghao Zhang, Yubin Ke, Alex K. -Y. Jen, Qiang Zhang, Xun-Li Wang, Qi Liu
Summary: The correlation between structure and function is crucial in materials science and engineering. Modern functional materials often exhibit inhomogeneities at the atomic level, giving them unique properties related to electrons, phonons, and magnetic moments. The pair distribution function (PDF) technique has emerged as a powerful tool for detecting local structure away from average in functional materials, with the advancements in crystallographic techniques and the availability of synchrotron X-rays, spallation neutrons, and advanced computing power.
Article
Pharmacology & Pharmacy
Vinicius D. N. Bezzon, Fabio F. Ferreira, Pamela Smith, Chris J. Benmore, Stephen R. Byrn, Gabriel L. B. de Araujo
Summary: X-ray pair distribution function (PDF) analysis is used to evaluate interactions and aging stability of amorphous solid dispersions, showing that ion-base interactions play a crucial role in reducing drug clustering processes.
INTERNATIONAL JOURNAL OF PHARMACEUTICS
(2021)
Article
Crystallography
Chuanbao Zheng, Hao Lu, Quanming Xu, Tianyi Liu, Aniruddha Patil, Jianyang Wu, Renko de Vries, Han Zuilhof, Zhisen Zhang
Summary: The polymorphism of ice is influenced by the crystalline substrates, with hexagonal ice being the dominant polymorph on graphene substrates. However, the preference for hexagonal ice diminishes as the ice layer grows.
Article
Chemistry, Multidisciplinary
Magnus Klove, Rasmus Stubkjaer Christensen, Ida Gjerlevsen Nielsen, Sanna Sommer, Mads Ry Vogel Jorgensen, Ann-Christin Dippel, Bo Brummerstedt Iversen
Summary: The structures of Zr4+ ions in solution were studied using X-ray pair distribution function (PDF) analysis. It was found that [Zr-4(OH)8(OH2)16]8+ tetramers are predominant in water, while monomeric complexes exist in non-aqueous solvents. The PDF analysis also revealed second sphere coordination of chloride counter ions to the aqueous tetramers.
Article
Chemistry, Multidisciplinary
Magnus Klove, Sanna Sommer, Bo B. Iversen, Bjork Hammer, Wilke Dononelli
Summary: A machine learning model incorporating density functional theory calculations and comparison of PDFs can be used to determine the crystal structure of unknown compounds, allowing for the identification of metastable configurations and stacking disorders.
ADVANCED MATERIALS
(2023)
Article
Materials Science, Multidisciplinary
Xiaoke Mu, Leyi Chen, Ralf Mikut, Horst Hahn, Christian Kubel
Summary: Amorphous nanophases are crucial for the properties of nanoscale heterogeneous materials, but experimental characterization of their atomic arrangement remains challenging. A new method is introduced to characterize local bonding and atomic packing in complex nanomaterials effectively.
Article
Chemistry, Physical
Roman D. Oparin, Michael A. Krestyaninov, Michael G. Kiselev
Summary: In this study, the conformational equilibria of lidocaine molecules in a saturated lidocaine solution in supercritical carbon dioxide (scCO2) under heating conditions were investigated. It was found that only conformers with an intramolecular hydrogen bond were realized within the studied range of state parameters. The solubility of lidocaine in scCO2 increased significantly with increasing temperature and density of the fluid phase, but did not lead to the formation of intermolecular hydrogen bonds. Heating changed the conformational equilibrium of lidocaine molecules in the scCO2 phase, but this change was not related to the destruction of intramolecular hydrogen bonds. Higher scCO2 phase density reduced the temperature effect on the conformational equilibrium. It was also observed that the temperature-induced conformational changes in lidocaine molecules in the scCO2 phase were reversible.
JOURNAL OF MOLECULAR LIQUIDS
(2022)
Article
Chemistry, Multidisciplinary
Justyna Grzonka, Marcel S. Claro, Alejandro Molina-Sanchez, Sascha Sadewasser, Paulo J. Ferreira
Summary: The new GaSe polymorph has a distinct atomic configuration and centrosymmetry, with its structure observed using electron microscopy and its stability confirmed through density-functional theory calculations. Predictions show slight differences in band structure and Raman intensities compared to known polymorphs.
ADVANCED FUNCTIONAL MATERIALS
(2021)
Article
Materials Science, Ceramics
Yu Zhou, Yong-chao Liang, Li-li Zhou, Yun-fei Mo, Reng-lai Wu, Ze-an Tian
Summary: With the development of high-pressure technology, the influence of pressure on the glass transition of zirconium (Zr) melt has been explored using molecular dynamics simulation. The results show that the glass transition temperature (Tg) and topologically close-packed (TCP) clusters increase with increasing pressure, leading to a reduction in configurational entropy. The second peak of the pair distribution function gradually shifts from the left to the right. Significant increases in A13[1/S444 10/S555 2/S666], Z12[12/S555], and Z14[12/S555 2/S666] clusters are observed under higher pressures, contributing to the splitting of the second peak in the distribution function.
JOURNAL OF NON-CRYSTALLINE SOLIDS
(2023)
Article
Chemistry, Multidisciplinary
Andy S. Anker, Troels Lindahl Christiansen, Marcus Weber, Martin Schmiele, Erik Brok, Emil T. S. Kjaer, Pavol Juhas, Rico Thomas, Michael Mehring, Kirsten M. O. Jensen
Summary: The study demonstrates the formation mechanism of metal oxido nanoclusters with a [Bi38O45] core using a combination of in situ pair distribution function (PDF) analysis and small-angle X-ray scattering (SAXS). The identification of [Bi22O26] as an intermediate species highlights the power of combined PDF and SAXS analysis for insights into nucleation on an atomic scale. Furthermore, the study shows how the interaction between nanoclusters and solvent is influenced by the nature of the ligands on the cluster surface.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Multidisciplinary
Zhu-Lin Xie, Xiaolin Liu, Andrew J. S. Valentine, Vincent M. Lynch, David M. Tiede, Xiaosong Li, Karen L. Mulfort
Summary: High-energy X-ray scattering and pair distribution function analysis is a powerful method for detecting the structure of molecular complexes in solution, revealing pairwise distances in local coordination spheres of metal centers and metal...metal distances. Comparing metal...metal distances detected in solution with crystal structure and molecular models can confirm unique distortions to metal bridging ligands in the solid state. This work demonstrates the potential for observing sub-angstrom conformational differences by comparing solution and solid-state structures directly.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Materials Science, Ceramics
Feng Li, Jingqi Zhang, Xinyu Xu, Hui Wang, Liang Feng, Hui Chang
Summary: In this study, molecular dynamics simulations were used to explain the splitting of the second peak in the pair distribution function (PDF) of Cu monatomic metallic glass (MG). The atomic packing in Cu MG exhibits a combination of spherical-periodic order and local translational symmetry. Voronoi tessellation analyses reveal that the dominant cluster is a crystal-like polyhedron <0, 3, 6, 4>. The splitting of the second peak is caused by the diverse connections between atomic clusters, with the first sub-peak originating from face-sharing clusters and the second sub-peak resulting from the alignment of central atoms and sharing atoms of vertex-sharing clusters.
JOURNAL OF NON-CRYSTALLINE SOLIDS
(2023)
Article
Chemistry, Applied
M. Asuncion Molina, Alicia Manjon-Sanz, Manuel Sanchez-Sanchez
Summary: In this study, a joint analysis of XRD and PDF was conducted on nanocrystalline M-MOF-74 materials, revealing the significance of PDF in studying nano-domains and providing information on crystal size range and slight structural deviations.
MICROPOROUS AND MESOPOROUS MATERIALS
(2021)
