Applications of pair distribution function methods to contemporary problems in materials chemistry

Young, Callum A.; Goodwin, Andrew L.

doi:10.1039/c0jm04415f

Cited by 140 publications

(121 citation statements)

References 118 publications

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“…PDF analysis is a long-established technique for studying the local structure of amorphous and disordered crystalline materials 11, 12 . To clarify the amorphous and crystalline phase fractions in the two coexisting phases, the differential PDF (d-PDF) method was used 13, 14 .…”

Section: Resultsmentioning

confidence: 99%

Pair distribution function analysis of sulfide glassy electrolytes for all-solid-state batteries: Understanding the improvement of ionic conductivity under annealing condition

Shiotani

Ohara

Tsukasaki

et al. 2017

Sci Rep

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In general, the ionic conductivity of sulfide glasses decreases with their crystallization, although it increases for a few sulphide glasses owing to the crystallization of a highly conductive new phase (e.g., Li7P3S11: 70Li2S-30P2S5). We found that the ionic conductivity of 75Li2S-25P2S5 sulfide glass, which consists of glassy and crystalline phases, is improved by optimizing the conditions of the heat treatment, i.e., annealing. A different mechanism of high ionic conductivity from the conventional mechanism is expected in the glassy phase. Here, we report the glassy structure of 75Li2S-25P2S5 immediately before the crystallization by using the differential pair distribution function (d-PDF) analysis of high-energy X-ray diffraction. Even though the ionic conductivity increases during the optimum annealing, the d-PDF analysis indicated that the glassy structure undergoes no structural change in the sulfide glass-ceramic electrolyte at a crystallinity of 33.1%. We observed the formation of a nanocrystalline phase in the X-ray and electron diffraction patterns before the crystallization, which means that Bragg peaks were deformed. Thus, the ionic conductivity in the mixture of glassy and crystalline phases is improved by the coexistence of the nanocrystalline phase.

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Section: Resultsmentioning

confidence: 99%

Pair distribution function analysis of sulfide glassy electrolytes for all-solid-state batteries: Understanding the improvement of ionic conductivity under annealing condition

Shiotani

Ohara

Tsukasaki

et al. 2017

Sci Rep

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“…However, the processes occurring during the formation of nanoparticles are not well understood, and this, to a large extent, prevents rational synthesis of new materials. [19][20][21][22][23][24] Because PDF analysis makes use of both Bragg and diffuse scattering intensities, it allows extraction of structural information from liquids, glasses, amorphous materials, nanocrystalline and disordered materials as well as crystalline structures. 7 This is known as the "nanostructure problem."…”

Section: Introductionmentioning

confidence: 99%

In situ total X-ray scattering study of the formation mechanism and structural defects in anatase TiO₂ nanoparticles under hydrothermal conditions

Jensen

Tyrsted

et al. 2015

CrystEngComm

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Polymorphism, morphology, particle size, and defects play key roles in the physical and chemical properties of nanoparticles. In hydrothermal synthesis of metal oxide nanoparticles, it is important to understand the influence of the specific precursor on these characteristics. Here, the formation mechanism of anatase TiO 2 nanoparticles by hydrolysis of titanium isopropoxide under hydrothermal conditions is studied by in situ total X-ray scattering and pair distribution function (PDF) analysis. It is shown that the amorphous precursor structure has short-range order up to~6.5 Å consisting of titanium hydroxide clusters made from TiO 6 /TiO 5 units in an arrangement related to anatase. Insight into the structural disorder of the anatase TiO 2 nanocrystals is obtained from both PDF and powder X-ray diffraction (PXRD)analyses. Defects of OH species are present on the surface of the nanocrystals, and their concentration correlates strongly with the particle size. Even though the formation of anatase TiO 2 under hydrothermal conditions resembles a solid-state phase transition from amorphous titania, the crystallization and grain growth kinetics of the nanocrystals are different due to the effects of the solvent. CrystEngCommThis journal is † Electronic supplementary information (ESI) available: Time evolution of in situ PXRD patterns; details and examples of the refinements of the PDFs of the ordered structure, the oxygen vacancy model, and OH defect model; details of the Rietveld refinement of the PXRD data; the oxygen z coordinate and the closest Ti-O distance as functions of reaction time; determination of the crystallinity of TiO 2 nanoparticles by PXRD. See

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“…9,24,[44][45][46] Total scattering is one of the few experimental techniques with simultaneous sensitivity to both average and local structure, 47,48 and so it is no accident that the two studies (of which we are aware) to attempt data-driven refinement of microscopic models of the orbital-disordered state are based on neutron total scattering measurements. 21,49 The first of these studies employed a "real-space Rietveld" (or "smallbox"; Ref.…”

Section: Orbital Correlations In the O Phasementioning

confidence: 99%

Local structure study of the orbital order/disorder transition inLaMnO3

et al. 2017

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We use a combination of neutron and X-ray total scattering measurements together with pair distribution function (PDF) analysis to characterise the variation in local structure across the orbital order-disorder transition in LaMnO3. Our experimental data are inconsistent with a conventional order-disorder description of the transition, and reflect instead the existence of a discontinuous change in local structure between ordered and disordered states. Within the orbital-ordered regime, the neutron and X-ray PDFs are best described by a local structure model with the same local orbital arrangements as those observed in the average (long-range) crystal structure. We show that a variety of meaningfully-different local orbital arrangement models can give fits of comparable quality to the experimental PDFs collected within the disordered regime; nevertheless, our data show a subtle but consistent preference for the anisotropic Potts model proposed in Phys Rev. B 79, 174106 (2009). The key implications of this model are electronic and magnetic isotropy together with the loss of local inversion symmetry at the Mn site. We conclude with a critical assessment of the interpretation of PDF measurements when characterising local symmetry breaking in functional materials.

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Applications of pair distribution function methods to contemporary problems in materials chemistry

Cited by 140 publications

References 118 publications

Pair distribution function analysis of sulfide glassy electrolytes for all-solid-state batteries: Understanding the improvement of ionic conductivity under annealing condition

Pair distribution function analysis of sulfide glassy electrolytes for all-solid-state batteries: Understanding the improvement of ionic conductivity under annealing condition

In situ total X-ray scattering study of the formation mechanism and structural defects in anatase TiO₂ nanoparticles under hydrothermal conditions

Local structure study of the orbital order/disorder transition inLaMnO3

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Applications of pair distribution function methods to contemporary problems in materials chemistry

Cited by 140 publications

References 118 publications

Pair distribution function analysis of sulfide glassy electrolytes for all-solid-state batteries: Understanding the improvement of ionic conductivity under annealing condition

Pair distribution function analysis of sulfide glassy electrolytes for all-solid-state batteries: Understanding the improvement of ionic conductivity under annealing condition

In situ total X-ray scattering study of the formation mechanism and structural defects in anatase TiO2 nanoparticles under hydrothermal conditions

Local structure study of the orbital order/disorder transition inLaMnO3

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In situ total X-ray scattering study of the formation mechanism and structural defects in anatase TiO₂ nanoparticles under hydrothermal conditions