A generalized solid-state nudged elastic band method

Sheppard, Daniel; Xiao, Penghao; Chemelewski, William D.; Johnson, Duane D.; Henkelman, Graeme

doi:10.1063/1.3684549

Cited by 771 publications

(602 citation statements)

References 15 publications

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“…The same acquisition and microscopy conditions were used for both phases. In addition to the observation of fine structure distinctions at the O‐K edge and Fe‐edges in the T ′ and S ′ domains, which will be discussed in detail elsewhere,33 low loss EELS provides local band structure information that can be compared to the first‐principles results. Figure 2b displays the spectra after background subtraction and plural scattering removal.…”

Section: Resultsmentioning

confidence: 99%

Understanding Strain‐Induced Phase Transformations in BiFeO₃ Thin Films

et al. 2015

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Experiments demonstrate that under large epitaxial strain a coexisting striped phase emerges in BiFeO3 thin films, which comprises a tetragonal‐like (T′) and an intermediate S′ polymorph. It exhibits a relatively large piezoelectric response when switching between the coexisting phase and a uniform T′ phase. This strain‐induced phase transformation is investigated through a synergistic combination of first‐principles theory and experiments. The results show that the S′ phase is energetically very close to the T′ phase, but is structurally similar to the bulk rhombohedral (R) phase. By fully characterizing the intermediate S′ polymorph, it is demonstrated that the flat energy landscape resulting in the absence of an energy barrier between the T′ and S′ phases fosters the above‐mentioned reversible phase transformation. This ability to readily transform between the S′ and T′ polymorphs, which have very different octahedral rotation patterns and c/a ratios, is crucial to the enhanced piezoelectricity in strained BiFeO3 films. Additionally, a blueshift in the band gap when moving from R to S′ to T′ is observed. These results emphasize the importance of strain engineering for tuning electromechanical responses or, creating unique energy harvesting photonic structures, in oxide thin film architectures.

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Section: Resultsmentioning

confidence: 99%

Understanding Strain‐Induced Phase Transformations in BiFeO₃ Thin Films

et al. 2015

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“…In order to investigate the profile of the BO surface in the vicinity of these two local minina and in the region that separates them we applied solid-state nudged-elastic band method. 27 Fig . 5 shows the minimum energy reaction path connecting the two minima and consisting of a concerted switch in the height of the Rb atoms with respect to the S elbow atoms occurring along with a change in the cell parameters.…”

Section: High Throughput Prediction Of the Structures Of Rbcus Anmentioning

confidence: 99%

Emergence of a few distinct structures from a single formal structure type during high-throughput screening for stable compounds: The case of RbCuS and RbCuSe

et al. 2015

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Theoretical sorting of stable and synthesizable "missing compounds" from those that are unstable is a crucial step in the discovery of previously unknown functional materials. This active research area often involves high throughput (HT) examination of the total energy of a given compound in a list of candidate formal structure types (FSTs), searching for those with the lowest energy within that list. While it is well appreciated that local relaxation methods based on a fixed list of structure types can lead to inaccurate geometries, this approach is widely used in HT studies because it produces answers faster than global optimization methods (that vary lattice vectors and atomic positions without local restrictions). We find, however a different failure mode of the HT protocol: specific crystallographic classes of formal structure types correspond each to a series of chemically distinct "daughter structure types" (DSTs) that have the same space group, but posses totally different local bonding configurations, including coordination types.Failure to include such DSTs in the fixed list of examined candidate structures used in contemporary high throughput approaches can lead to qualitative misidentification of the stable bonding pattern, not just quantitative inaccuracies. In this work we (i) clarify the understanding of the general DST-FST relationship, thus improving current discovery HT approaches, (ii) illustrate this failure mode for RbCuS and RbCuSe (a newly predicted compound) by developing a synthesis method and accelerated crystal structure determination and, (iii) apply the genetic-algorithm based Global Space Group Optimization (GSGO) approach which is not vulnerable to the failure-mode of HT searches of fixed lists, demonstrating a correct identification of the stable DST. The broad impact of items (i)-(iii) lies in the demonstrated understanding of a new strategy-use HT as preliminary broad screening, followed by unbiased GSGO of the final candidates.2

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“…Here, we adopt an analogous approach to ref. 36 and obtain a generalization of the (D)NEB method for a system of rigid bodies that involve translational and rotational coordinates.…”

Section: Chain Of State Methodsmentioning

confidence: 99%

Exploring Energy Landscapes: Metrics, Pathways, and Normal-Mode Analysis for Rigid-Body Molecules

Rühle

Kusumaatmaja

Chakrabarti

et al. 2013

J. Chem. Theory Comput.

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We present new methodology for exploring the energy landscapes of molecular systems, using angle-axis variables for the rigid-body rotational coordinates. The key ingredient is a distance measure or metric tensor, which is invariant to global translation and rotation. The metric is used to formulate a generalized nudged elastic band method for calculating pathways, and a full prescription for normal-mode analysis is described. The methodology is tested by mapping the potential energy and free energy landscape of the water octamer, described by the TIP4P potential.

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A generalized solid-state nudged elastic band method

Cited by 771 publications

References 15 publications

Understanding Strain‐Induced Phase Transformations in BiFeO₃ Thin Films

Understanding Strain‐Induced Phase Transformations in BiFeO₃ Thin Films

Emergence of a few distinct structures from a single formal structure type during high-throughput screening for stable compounds: The case of RbCuS and RbCuSe

Exploring Energy Landscapes: Metrics, Pathways, and Normal-Mode Analysis for Rigid-Body Molecules

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A generalized solid-state nudged elastic band method

Cited by 771 publications

References 15 publications

Understanding Strain‐Induced Phase Transformations in BiFeO3 Thin Films

Understanding Strain‐Induced Phase Transformations in BiFeO3 Thin Films

Emergence of a few distinct structures from a single formal structure type during high-throughput screening for stable compounds: The case of RbCuS and RbCuSe

Exploring Energy Landscapes: Metrics, Pathways, and Normal-Mode Analysis for Rigid-Body Molecules

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Product

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Understanding Strain‐Induced Phase Transformations in BiFeO₃ Thin Films

Understanding Strain‐Induced Phase Transformations in BiFeO₃ Thin Films