<i>Ab initio</i> random structure searching of organic molecular solids: assessment and validation against experimental data

Zilka, Miri; Dudenko, Dmytro; Hughes, Colan E.; Williams, P. Andrew; Sturniolo, Simone; Franks, W. Trent; Pickard, Chris J.; Yates, Jonathan R.; Harris, Kenneth D. M.; Brown, Steven P.

doi:10.1039/c7cp04186a

Cited by 28 publications

(26 citation statements)

References 84 publications

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“…Although in principle the number of structures that can be searched is restricted by the higher cost of DFT (in comparison to cheaper force-field approaches), the unbiased nature of the method has significant advantages for inorganic systems and for predicting higher-energy (but perhaps still experimentally relevant) structures. AIRSS has been combined with the calculation of NMR parameters to study battery materials (e.g., identifying the structure of previously-unknown structures of Li/Ge phases 54 ), silicate minerals (e.g., locating the position of H in high-pressure materials of relevance in the inner Earth 55 ), and organic molecules (e.g., to study possible polymorphism 56 ). Figure 4 shows the energy of AIRSS-predicted structures of potential Na-Sn based anode materials as a function of composition.…”

Section: Exploiting Resolution For Nmr Crystallographymentioning

confidence: 99%

Perspective: Current advances in solid-state NMR spectroscopy

Ashbrook

Hodgkinson

2018

The Journal of Chemical Physics

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In contrast to the rapid and revolutionary impact of solution-state Nuclear Magnetic Resonance (NMR) on modern chemistry, the field of solid-state NMR has matured more slowly. This reflects the major technical challenges of much reduced spectral resolution and sensitivity in solid-state as compared to solution-state spectra, as well as the relative complexity of the solid state. In this perspective, we outline the technique developments that have pushed resolution to intrinsic limits and the approaches, including ongoing major developments in the field of Dynamic Nuclear Polarisation, that have enhanced spectral sensitivity. The information on local structure and dynamics that can be obtained using these gains in sensitivity and resolution is illustrated with a diverse range of examples from large biomolecules to energy materials and pharmaceuticals and from both ordered and highly disordered materials. We discuss how parallel developments in quantum chemical calculation, particularly density functional theory, have enabled experimental data to be translated directly into information on local structure and dynamics, giving rise to the developing field of "NMR crystallography."

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Section: Exploiting Resolution For Nmr Crystallographymentioning

confidence: 99%

Perspective: Current advances in solid-state NMR spectroscopy

Ashbrook

Hodgkinson

2018

The Journal of Chemical Physics

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“…The combination of CSP and calculating (nonthermodynamic) properties, whether for targeting new functional materials or for structural characterisation, such as various diffraction 78 or solid state NMR experiments, 79 is really contributing to science. The question though is how much this relies on human scientic understanding interpreting the results of the CSP_0 (or CSP_thd) for experimental collaborators, or whether we can have a black-box computer code.…”

Section: 77mentioning

confidence: 99%

Is zeroth order crystal structure prediction (CSP_0) coming to maturity? What should we aim for in an ideal crystal structure prediction code?

Price

2018

Faraday Discuss.

117

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Crystal structure prediction based on searching for the global minimum in the lattice energy (CSP_0) is growing in use for guiding the discovery of new materials, for example, new functional materials, new phases of interest to planetary scientists and new polymorphs relevant to pharmaceutical development. This Faraday Discussion can assess the progress of CSP_0 over the range of types of materials to which CSP is currently and could be applied, which depends on our ability to model the variety of interatomic forces in crystals. The basic hypothesis, that the outcome of crystallisation is determined by thermodynamics, needs examining by considering methods of modelling relative thermodynamic stability not only as a function of pressure and temperature, but also of size, solvent and the presence of heterogeneous templates or impurities (CSP_thd). Given that many important materials persist, and indeed may be formed, when they are not the most thermodynamically stable structure, we need to define what would be required of an ideal CSP code (CSP_aim).

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“…Solid‐state nuclear magnetic resonance (ssNMR) is one of the most important analytical tools providing atomically resolved information on the molecular and crystal structure of solid materials. Recent developments in ssNMR involving the available high‐field NMR systems and specialized pulse sequences enabled the use of multinuclear solid‐state NMR spectroscopy in combination with density functional theory (DFT) calculations to be widely applied for structure determination and validation of organic molecular compounds . Although ssNMR spectroscopy is ideally suited for in‐depth, atomic resolution analysis, some experiments on many APIs still suffer from poor sensitivity.…”

Section: Introductionmentioning

confidence: 99%

Identifying aspirin polymorphs from combined DFT‐based crystal structure prediction and solid‐state NMR

Mathew

Uchman

Gkoura

et al. 2020

Magnetic Reson in Chemistry

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A combined experimental and computational approach was used to distinguish between different polymorphs of the pharmaceutical drug aspirin. This method involves the use of ab initio random structure searching (AIRSS), a density functional theory (DFT)-based crystal structure prediction method for the high-accuracy prediction of polymorphic structures, with DFT calculations of nuclear magnetic resonance (NMR) parameters and solid-state NMR experiments at natural abundance. AIRSS was used to predict the crystal structures of form-I and form-II of aspirin. The root-mean-square deviation between experimental and calculated 1 H chemical shifts was used to identify form-I as the polymorph present in the experimental sample, the selection being successful despite the large similarities between the molecular environments in the crystals of the two polymorphs.

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Ab initio random structure searching of organic molecular solids: assessment and validation against experimental data

Abstract: The AIRSS method generates crystal structures for m-aminobenzoic acid; comparison is made to experimental powder X-ray diffraction and MAS NMR.

Cited by 28 publications

References 84 publications

Perspective: Current advances in solid-state NMR spectroscopy

Perspective: Current advances in solid-state NMR spectroscopy

Is zeroth order crystal structure prediction (CSP_0) coming to maturity? What should we aim for in an ideal crystal structure prediction code?

Identifying aspirin polymorphs from combined DFT‐based crystal structure prediction and solid‐state NMR

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