2021 New's Items

Benchmarking Coordination Number Prediction Algorithms on Inorganic Crystal Structures

Pan H
Ganose AM
Horton M
Aykol M
Persson KA
Zimmermann NER
Jain A
2021

Coordination numbers and geometries form a theoretical framework for understanding and predicting materials properties. Algorithms to determine coordination numbers automatically are increasingly used for machine learning (ML) and automatic structural analysis. In this work, we introduce MaterialsCoord, a benchmark suite containing 56 experimentally derived crystal structures (spanning elements, binaries, and ternary compounds) and their corresponding coordination environments as described in the research literature. We also describe CrystalNN, a novel algorithm for determining near...

Automated Adsorption Workflow for Semiconductor Surfaces and the Application to Zinc Telluride

Andriuc O
Siron M
Montoya JH
Horton M
Persson KA
2021

Surface adsorption is a crucial step in numerous processes, including heterogeneous catalysis, where the adsorption of key species is often used as a descriptor of efficiency. We present here an automated adsorption workflow for semiconductors which employs density functional theory calculations to generate adsorption data in a high-throughput manner. Starting from a bulk structure, the workflow performs an exhaustive surface search, followed by an adsorption structure construction step, which generates a minimal energy landscape to determine the optimal adsorbate–surface distance....

Aqueous Stability of Zirconium Clusters, Including the Zr(IV) Hexanuclear Hydrolysis Complex [Zr6O4(OH)4(H2O)24]12+, from Density Functional Theory

Stern RD
Kingsbury RS
Persson KA
2021

Framework materials constitute a broad family of solids that range from zeolites and metal–organic frameworks (MOFs) to coordination polymers. The synthesis of such network structures typically rely on precursor molecular building blocks. As an example, the UiO-66 MOF series is constructed of hexanuclear [Zr6O4(OH)4(CO2)12] cluster nodes and linear carboxylate linkers. Unfortunately, these Zr MOF cluster nodes cannot currently be manufactured in a...

Advancing Electrolyte Solution Chemistry and Interfacial Electrochemistry of Divalent Metal Batteries

Wang H
Ryu J
Shao Y
Murugesan V
Persson K
Zavadil K
Mueller KT
Liu J
2021

Divalent metal (Mg, Ca, etc.) battery chemistries potentially provide a sustainable long-term technical solution for large-scale energy storage because of the high natural abundance of divalent metal elements in the earth crust. Good progress has been made on materials especially electrolyte development in the past years; however, significant challenges exist, particularly the very limited fundamental understanding of electrolyte solution chemistry and interfacial electrochemistry. In this perspective, we review and discuss key discoveries and understanding of divalent battery...

A graph-based network for predicting chemical reaction pathways in solid-state materials synthesis

McDermott MJ
Dwaraknath SS
Persson KA
2021

Accelerated inorganic synthesis remains a significant challenge in the search for novel, functional materials. Many of the principles which enable “synthesis by design” in synthetic organic chemistry do not exist in solid-state chemistry, despite the availability of extensive computed/experimental thermochemistry data. In this work, we present a chemical reaction network model for solid-state synthesis constructed from available thermochemistry data and devise a computationally tractable approach for suggesting likely reaction pathways via the application of pathfinding algorithms...

A framework for quantifying uncertainty in DFT energy corrections

Wang A
Kingsbury R
McDermott M
Horton M 2
Jain A
Ong PS
Dwaraknath S
Persson KA
2021

In this work, we demonstrate a method to quantify uncertainty in corrections to density functional theory (DFT) energies based on empirical results. Such corrections are commonly used to improve the accuracy of computational enthalpies of formation, phase stability predictions, and other energy-derived properties, for example. We incorporate this method into a new DFT energy correction scheme comprising a mixture of oxidation-state and composition-dependent corrections and show that many chemical systems contain unstable polymorphs that may actually be predicted stable when...

Full spectrum optical constant interface to the Materials Project

Kas JJ
Vila FD
Pemmaraju CD
Persson KA
Prang PM
Yang RX
Rehr JJ
2021

Optical constants characterize the interaction of materials with light and are important properties in material design. Here we present a Python-based Corvus workflow for simulations of full spectrum optical constants from the visible and ultraviolet to hard x-ray wavelengths based on the real-space Green’s function code FEFF10 and structural data from the Materials Project (MP). The Corvus workflow manager and its associated tools provide an interface to FEFF10 and the MP database. The workflow parallelizes the FEFF computations of optical constants over all absorption edges for...

Transport Phenomena in Low Temperature Lithium-Ion Battery Electrolytes

Ringsby AJ
Fong KD
Self J
Bergstrom HK
McCloskey BD
Persson KA
2021

Lithium-ion batteries face low temperature performance issues, limiting the adoption of technologies ranging from electric vehicles to stationary grid storage. This problem is thought to be exacerbated by slow transport within the electrolyte, which in turn may be influenced by ion association, solvent viscosity, and cation transference number. How these factors collectively impact low temperature transport phenomena, however, remains poorly understood. Here we show using all-atom classical molecular dynamics (MD) simulations that the dominant factor influencing low temperature...

The solvation structure, transport properties and reduction behavior of carbonate-based electrolytes of lithium-ion batteries

Hou T
Fong KD
Wang J
Persson KA
2021

Despite the extensive employment of binary/ternary mixed-carbonate electrolytes (MCEs) for Li-ion batteries, the role of each ingredient with regards to the solvation structure, transport properties, and reduction behavior is not fully understood. Herein, we report the atomistic modeling and transport property measurements of the Gen2 (1.2 M LiPF6 in ethylene carbonate (EC) and ethyl methyl carbonate (EMC)) and EC-base (1.2 M LiPF6 in EC) electrolytes, as well as their mixtures with 10 mol%...

Phase-contrast imaging of multiply-scattering extended objects at atomic resolution by reconstruction of the scattering matrix

Philipp M. Pelz
Hamish G. Brown
Scott Stonemeyer
Scott D. Findlay
Alex Zettl
Peter Ercius
Yaqian Zhang
Jim Ciston
M. C. Scott
Colin Ophus
2021

Three-dimensional phase-contrast imaging of multiply-scattering samples in x-ray and electron microscopy is challenging due to small numerical apertures, the unavailability of wave front shaping optics, and the highly nonlinear inversion required from intensity-only measurements. In this work, we present an algorithm using the scattering matrix formalism to solve the scattering from a noncrystalline medium from scanning diffraction measurements and simultaneously recover the illumination aberrations. We demonstrate our method experimentally in a scanning transmission electron...