Opportunities and challenges in understanding complex functional materials

Goodwin, Andrew L.

doi:10.1038/s41467-019-12422-z

Cited by 39 publications

(37 citation statements)

References 15 publications

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“…COMMUNICATIONS CHEMISTRY | https://doi.org/10.1038/s42004-020-0269-2 ARTICLE COMMUNICATIONS CHEMISTRY | (2020) 3:22 | https://doi.org/10.1038/s42004-020-0269-2 | www.nature.com/commschem information content in scattering data and imposes strong constraints on refinement 17 . Moreover, nanocomposite materials are inherently non-equilibrium phases, which in turn complicates the application of conventional computational methodologies to structural modelling.…”

Section: Discussionmentioning

confidence: 99%

“…In this respect, ferrihydrite is representative of an important general challenge facing structural science: namely, how might we develop robust protocols for determining the structure of nanoscale materials [15][16][17] ? The conventional-and most straightforwardapproach is to approximate nanomaterials as periodic crystals modified by a suitable shape function.…”

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Nanocomposite structure of two-line ferrihydrite powder from total scattering

et al. 2020

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Ferrihydrite is one of the most important iron-containing minerals on Earth. Yet determination of its atomic-scale structure has been frustrated by its intrinsically poor crystallinity. The key difficulty is that physically-different models can appear consistent with the same experimental data. Using X-ray total scattering and a nancomposite reverse Monte Carlo approach, we evaluate the two principal contending models-one a multi-phase system without tetrahedral iron(III), and the other a single phase with tetrahedral iron(III). Our methodology is unique in considering explicitly the complex nanocomposite structure the material adopts: namely, crystalline domains embedded in a poorly-ordered matrix. The multi-phase model requires unphysical structural rearrangements to fit the data, whereas the single-phase model accounts for the data straightforwardly. Hence the latter provides the more accurate description of the short-and intermediate-range order of ferrihydrite. We discuss how this approach might allow experiment-driven (in)validation of complex models for important nanostructured phases beyond ferrihydrite.

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Section: Discussionmentioning

confidence: 99%

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Nanocomposite structure of two-line ferrihydrite powder from total scattering

et al. 2020

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“…Thanks to a meticulous control over synthesis conditions and an ever‐expanding versatile set of experimentally available building blocks, it has even become possible to synthesize combinations of building blocks in different structures. To fully explore the functionalities of the enormous amount of potential structures that can be formed from a given set of building blocks, an accurate protocol is needed to systematically derive structural models for these materials at realistic working conditions of temperature and pressure [16, 17] . Such structural characterization is a conditio sine qua non for the atomically guided design of functional applications in the fields of catalysis, sorption, light harvesting and more.…”

Section: Introductionmentioning

confidence: 99%

Quantifying the Likelihood of Structural Models through a Dynamically Enhanced Powder X‐Ray Diffraction Protocol

et al. 2021

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Structurally characterizing new materials is tremendously challenging,especially when single crystal structures are hardly available which is often the case for covalent organic frameworks.Y et, knowledge of the atomic structure is key to establish structure-function relations and enable functional material design. Herein, an ew protocol is proposed to unambiguously predict the structure of poorly crystalline materials through al ikelihood ordering based on the X-ray diffraction (XRD) pattern. Keyo fthep rocedure is the broad set of structures generated from al imited number of building blocks and topologies,w hichi ss ubmitted to operando structural characterization. The dynamic averaging in the latter accounts for the operando conditions and inherent temporal character of experimental measurements,y ielding unparalleled agreement with experimental powder XRD patterns.T he proposed concept can hence unquestionably identify the structure of experimentally synthesized materials, ac rucial step to design next generation functional materials.

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“…In many functional materials, from leading ferroelectric [8][9][10] and thermoelectric candidates [11][12][13] to photovoltaic perovskites [14] and ionic conductors [15], correlated deviation from perfect periodicity plays a pivotal role in governing functionality. This is the purview of disorder engineering; controlling the disorder within a system to create materials with new or improved functionality [16].…”

Section: Introductionmentioning

confidence: 99%

Tuneable correlated disorder in alloys

Chaney

Castellano

Bosak

et al. 2021

Phys. Rev. Materials

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Understanding the role of disorder, and the correlations that exist within it, is one of the defining challenges in contemporary materials science. However, there are few material systems, devoid of other complex interactions, that can be used to systematically study the effects of crystallographic conflict on correlated disorder. Here, we report extensive diffuse x-ray scattering studies on the epitaxially stabilized alloy U 1−x Mo x , showing that a new form of intrinsically tuneable correlated disorder arises from a mismatch between the preferred symmetry of a crystallographic basis and the lattice upon which it is arranged. Furthermore, combining grazing incidence inelastic x-ray scattering and state-of-the-art ab initio molecular dynamics simulations, we discover strong disorder-phonon coupling. This breaks global symmetry and dramatically suppresses phonon lifetimes compared to alloying alone, providing an additional design strategy for phonon engineering. These findings have implications wherever crystallographic conflict can be accommodated, and they may be exploited in the development of future functional materials.

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Opportunities and challenges in understanding complex functional materials

Cited by 39 publications

References 15 publications

Nanocomposite structure of two-line ferrihydrite powder from total scattering

Nanocomposite structure of two-line ferrihydrite powder from total scattering

Quantifying the Likelihood of Structural Models through a Dynamically Enhanced Powder X‐Ray Diffraction Protocol

Tuneable correlated disorder in alloys

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