Evaluation of nano- and mesoscale structural features in composite materials through hierarchical decomposition of the radial distribution function

Composite materials possessing both crystalline and amorphous domains, when subjected to X-ray and neutron scattering, generate diffraction patterns that are often difficult to interpret. One approach is to perform atomistic simulations of a proposed structure, from which the analogous diffraction pattern can be obtained for validation. The structure can be iteratively refined until simulation and experiment agree. The practical drawback to this approach is the significant computational resources required for the simulations. In this work, an alternative approach based on a hierarchical decomposition of the radial distribution function is used to generate a physics-based model allowing rapid interpretation of scattering data. In order to demonstrate the breadth of this approach, it is applied to a series of carbon composites. The model is compared with atomistic simulation results in order to demonstrate that the contributions of the crystalline and amorphous domains, as well as their interfaces, are correctly captured. Because the model is more efficient, additional structural refinement is performed to increase the agreement of the simulation result with the experimental data. The model achieves a reduction in computational effort of six orders of magnitude relative to simulation. The model can be generally extended to other composite materials.

[1]  L. Martin-Gondre,et al.  Modeling the THF clathrate hydrate dynamics by combining molecular dynamics and quasi-elastic neutron scattering , 2017 .

[2]  Thomas Proffen,et al.  An automated analysis workflow for optimization of force-field parameters using neutron scattering data , 2017, J. Comput. Phys..

[3]  T. Grande,et al.  Local Structure of Disordered Bi0.5K0.5TiO3 Investigated by Pair Distribution Function Analysis and First-Principles Calculations , 2017 .

[4]  O. Rios,et al.  Li-Ion Localization and Energetics as a Function of Anode Structure. , 2017, ACS applied materials & interfaces.

[5]  Kamal B. Dhungana,et al.  Structure of cyano-anion ionic liquids: X-ray scattering and simulations. , 2016, The Journal of chemical physics.

[6]  O. Rios,et al.  Hierarchical Model for the Analysis of Scattering Data of Complex Materials , 2016 .

[7]  K. Page,et al.  DShaper: an approach for handling missing low‐Q data in pair distribution function analysis of nanostructured systems , 2015 .

[8]  Zhanhu Guo,et al.  Polymer nanocomposites for energy storage, energy saving, and anticorrosion , 2015 .

[9]  K. Winey,et al.  Direct Comparisons of X-ray Scattering and Atomistic Molecular Dynamics Simulations for Precise Acid Copolymers and Ionomers , 2015 .

[10]  Andrew H. Van Benschoten,et al.  Conformational dynamics of a crystalline protein from microsecond-scale molecular dynamics simulations and diffuse X-ray scattering , 2014, Proceedings of the National Academy of Sciences.

[11]  T. Proffen,et al.  Structural analysis of lignin-derived carbon composite anodes , 2014 .

[12]  Dean A. J. Whittaker,et al.  High-pressure transformation of SiO₂ glass from a tetrahedral to an octahedral network: a joint approach using neutron diffraction and molecular dynamics. , 2014, Physical review letters.

[13]  D. Miklavčič,et al.  Structural properties of archaeal lipid bilayers: small-angle X-ray scattering and molecular dynamics simulation study. , 2014, Langmuir : the ACS journal of surfaces and colloids.

[14]  O. Diat,et al.  Elucidation of the structure of organic solutions in solvent extraction by combining molecular dynamics and X-ray scattering. , 2014, Angewandte Chemie.

[15]  Rosemary K. Le,et al.  Analysis of the solution structure of Thermosynechococcus elongatus photosystem I in n-dodecyl-β-D-maltoside using small-angle neutron scattering and molecular dynamics simulation. , 2014, Archives of biochemistry and biophysics.

[16]  O. Rios,et al.  Entropy-driven structure and dynamics in carbon nanocrystallites , 2014, Journal of Nanoparticle Research.

[17]  T. Darling,et al.  Quantifying amorphous and crystalline phase content with the atomic pair distribution function , 2013 .

[18]  Anders Nilsson,et al.  Benchmark oxygen-oxygen pair-distribution function of ambient water from x-ray diffraction measurements with a wide Q-range. , 2013, The Journal of chemical physics.

[19]  I. Levin,et al.  Reverse Monte Carlo refinements of nanoscale atomic correlations using powder and single-crystal diffraction data , 2012 .

[20]  Bryan W. Holland,et al.  Scattering density profile model of POPG bilayers as determined by molecular dynamics simulations and small-angle neutron and X-ray scattering experiments. , 2012, The journal of physical chemistry. B.

[21]  P. McMillan,et al.  Polyamorphic amorphous silicon at high pressure: raman and spatially resolved X-ray scattering and molecular dynamics studies. , 2011, The journal of physical chemistry. B.

[22]  Jeremy C. Smith,et al.  Self-similar multiscale structure of lignin revealed by neutron scattering and molecular dynamics simulation. , 2011, Physical review. E, Statistical, nonlinear, and soft matter physics.

[23]  K. Amine,et al.  Combining the pair distribution function and computational methods to understand lithium insertion in Brookite (TiO2). , 2011, Inorganic chemistry.

[24]  K. Chapman,et al.  Elucidating the structure of surface acid sites on γ-Al2O3. , 2011, Journal of the American Chemical Society.

[25]  A. Bytchkov,et al.  The structure of liquid calcium aluminates as investigated using neutron and high energy x-ray diffraction in combination with molecular dynamics simulation methods , 2011, Journal of physics. Condensed matter : an Institute of Physics journal.

[26]  T. Proffen,et al.  Building and refining complete nanoparticle structures with total scattering data , 2011 .

[27]  R. Atkin,et al.  Amphiphilicity determines nanostructure in protic ionic liquids. , 2011, Physical chemistry chemical physics : PCCP.

[28]  S. A. Kori,et al.  Defence Applications of Polymer Nanocomposites , 2010 .

[29]  Jincheng Du,et al.  A molecular dynamics simulation interpretation of neutron and x-ray diffraction measurements on single phase Y2O3–Al2O3 glasses , 2009, Journal of physics. Condensed matter : an Institute of Physics journal.

[30]  Thomas Proffen,et al.  Neutron powder diffraction and molecular simulation study of the structural evolution of ammonia borane from 15 to 340 K. , 2009, The journal of physical chemistry. A.

[31]  Reinhard B. Neder,et al.  Diffuse Scattering and Defect Structure Simulations: A Cook Book Using the Program DISCUS , 2009 .

[32]  Gonzalo Gutiérrez,et al.  Structural and vibrational properties of amorphous GeO2: a molecular dynamics study , 2008 .

[33]  S J L Billinge,et al.  PDFfit2 and PDFgui: computer programs for studying nanostructure in crystals , 2007, Journal of physics. Condensed matter : an Institute of Physics journal.

[34]  P. Woodward,et al.  Local Atomic Ordering in BaTaO2N Studied by Neutron Pair Distribution Function Analysis and Density Functional Theory , 2007 .

[35]  Qun Hui,et al.  RMCProfile: reverse Monte Carlo for polycrystalline materials , 2007, Journal of physics. Condensed matter : an Institute of Physics journal.

[36]  Jincheng Du,et al.  Understanding lanthanum aluminate glass structure by correlating molecular dynamics simulation results with neutron and X-ray scattering data , 2007 .

[37]  M. Bellissent-Funel,et al.  Local order in aqueous NaCl solutions and pure water: X-ray scattering and molecular dynamics simulations study. , 2006, The journal of physical chemistry. B.

[38]  Simon J. L. Billinge,et al.  PDFgetX2: a GUI-driven program to obtain the pair distribution function from X-ray powder diffraction data , 2004 .

[39]  K. Hermansson,et al.  X-ray and neutron diffraction studies and molecular dynamics simulations of liquid DMSO , 2004 .

[40]  Simon J. L. Billinge,et al.  Underneath the Bragg Peaks: Structural Analysis of Complex Materials , 2003 .

[41]  Matthias Krack,et al.  Water structure as a function of temperature from X-ray scattering experiments and ab initio molecular dynamics , 2003 .

[42]  M. Mezouar,et al.  Quantitative structure factor and density measurements of high-pressure fluids in diamond anvil cells by x-ray diffraction: Argon and water , 2002 .

[43]  Gonzalo Gutiérrez,et al.  Molecular dynamics study of structural properties of amorphous Al 2 O 3 , 2002 .

[44]  Martin T. Dove,et al.  Application of the reverse Monte Carlo method to crystalline materials , 2001 .

[45]  K. Hermansson,et al.  Hydration of the calcium ion. An EXAFS, large-angle x-ray scattering, and molecular dynamics simulation study. , 2001, Journal of the American Chemical Society.

[46]  Simon J. L. Billinge,et al.  PDFFIT, a program for full profile structural refinement of the atomic pair distribution function , 1999 .

[47]  T. Proffen,et al.  DISCUS: a program for diffuse scattering and defect‐structure simulation , 1997 .

[48]  S. D. Smith,et al.  Molecular dynamics simulation of atactic polystyrene. 2. Comparison with neutron scattering data , 1994 .

[49]  V. Maroulas,et al.  Interfacial Li-ion localization in hierarchical carbon anodes , 2017 .

[50]  P. Fulvio,et al.  Densification of Ionic Liquid Molecules within a Hierarchical Nanoporous Carbon Structure Revealed by Small-Angle Scattering and Molecular Dynamics Simulation , 2014 .

[51]  O. Rios,et al.  Highly Robust Lithium Ion Battery Anodes from Lignin: An Abundant, Renewable, and Low‐Cost Material , 2014 .

[52]  Lloyd L. Lee,et al.  Molecular Thermodynamics of Nonideal Fluids , 1988 .