A high-throughput infrastructure for density functional theory calculations

Jain, Anubhav; Hautier, Geoffroy; Moore, Christopher; Ong, Shyue Ping; Fischer, Curt R.; Mueller, Tim; Persson, Kristin A.; Ceder, Gerbrand

doi:10.1016/j.commatsci.2011.02.023

Cited by 958 publications

(901 citation statements)

References 86 publications

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“…Approximate density functional theory (DFT) remains the method of choice for computational discovery [4][5][6][7][8][9][10][11] , owing to its favorable balance of accuracy and efficiency. 12 Nevertheless, delocalization errors [13][14] and other biases in semi-local exchange approximations [15][16] (e.g., the generalized gradient approximation or GGA) produce systematic biases toward low-spin states [17][18] that prevent prediction of either qualitative (i.e., ground state identity) or quantitative (i.e., energetic splitting between states) spin-state properties.…”

Section: Introductionmentioning

confidence: 99%

Ligand-Field-Dependent Behavior of Meta-GGA Exchange in Transition-Metal Complex Spin-State Ordering

2017

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Prediction of spin-state ordering in transition metal complexes is essential for understanding catalytic activity and designing functional materials. Semi-local approximations in density functional theory, such as the generalized-gradient approximation (GGA), suffer from several errors notably including delocalization error that give rise to systematic bias for more covalently bound low-spin electronic states. Incorporation of exact exchange is known to counteract this bias, instead favoring high-spin states, in a manner that has recently been identified to be ligand-field dependent. In this work, we introduce a tuning strategy to identify the effect of incorporating the Laplacian of the density (i.e., a meta-GGA) in exchange on spinstate ordering. We employ a diverse test set of M(II) and M(III) first-row transition metal ions from Ti to Cu as well as octahedral complexes of these ions with ligands of increasing field strength (i.e., H 2 O, NH 3 , and CO). We show that the sensitivity of spin-state ordering to meta-GGA exchange is highly ligand-field dependent, stabilizing high-spin states in strong-field (i.e., CO) cases and stabilizing low-spin states in weak-field (i.e., H 2 O, NH 3 , and isolated ions) cases. This diverging behavior leads to generally improved treatment of isolated ions and strong field complexes over a standard GGA but worsened treatment for the hexa-aqua or hexa-ammine complexes. These observations highlight the sensitivity of functional performance to subtle changes in chemical bonding.2

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Section: Introductionmentioning

confidence: 99%

Ligand-Field-Dependent Behavior of Meta-GGA Exchange in Transition-Metal Complex Spin-State Ordering

2017

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“…[17]). The HT approach has been used to find new materials and trends with data-mining algorithms [10,11,[18][19][20][21]. As an example, Madsen reported an ab-initio search for thermoelectrics containing Zn and Sb [22].…”

Section: Introductionmentioning

confidence: 99%

Assessing the Thermoelectric Properties of Sintered Compounds via High-ThroughputAb-InitioCalculations

et al. 2011

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Several thousand compounds from the Inorganic Crystal Structure Database have been considered as nanograined, sintered-powder thermoelectrics with the high-throughput ab-initio AFLOW framework. Regression analysis unveils that the power factor is positively correlated with both the electronic band gap and the carrier effective mass, and that the probability of having large thermoelectric power factors increases with the increasing number of atoms per primitive cell. Avenues for further investigation are revealed by this work. These avenues include the role of experimental and theoretical databases in the development of novel materials.

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“…MD simulations present an extreme example, where multiweek runs well in excess of the wall times of most supercomputing resources are typical. A recent trend in computational materials science has been the development of high-throughput infrastructures [158][159][160][161][162] that can perform 'standardized' calculations over hundreds to thousands of materials. Such software developments will surely lower the barrier for computational investigations of alkali diffusion.…”

Section: Computational Studies Of Alkali Conduction Z Deng Et Almentioning

confidence: 99%

Computational studies of solid-state alkali conduction in rechargeable alkali-ion batteries

Deng

Ong

2016

NPG Asia Mater

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The facile conduction of alkali ions in a crystal host is of crucial importance in rechargeable alkali-ion batteries, the dominant form of energy storage today. In this review, we provide a comprehensive survey of computational approaches to study solid-state alkali diffusion. We demonstrate how these methods have provided useful insights into the design of materials that form the main components of a rechargeable alkali-ion battery, namely the electrodes, superionic conductor solid electrolytes and interfaces. We will also provide a perspective on future challenges and directions. The scope of this review includes the monovalent lithium-and sodium-ion chemistries that are currently of the most commercial interest. NPG Asia Materials (2016) 8, e254; doi:10.1038/am.2016.7; published online 25 March 2016 INTRODUCTIONThe facile conduction of alkali ions in a crystal is of critical importance in energy storage. Today, the dominant form of energy storage in consumer electronics is the rechargeable lithium-ion (Li-ion) battery, 1-5 a device that functions entirely on the basis of the reversible transport of Li + ions. With one of the highest energy densities of known energy storage technologies, Li-ion batteries are finding increasingly large-scale applications in electrified transportation and grid storage. In recent years, there has also been a resurgence of interest in rechargeable sodium-ion (Na-ion) batteries, 6-12 which function on the same basic principle but with Na + instead of Li + because of concerns regarding the abundance and cost of lithium. Figure 1 shows a representation of a rechargeable alkali-ion battery. The typical electrode in an alkali-ion battery is an intercalation compound, which, as the name implies, stores alkali ions by inserting them into its crystal structure in a topotactic manner. During discharge, A + ions are transported from the anode, through the electrolyte and into the cathode. The reverse happens during charge. Throughout this review, we will adopt the customary terminology of defining the 'cathode' as the positive electrode during discharge, even though the formal definition of the cathode changes depending on whether the charging or discharging process is being referred to. Current cathodes are typically transition metal oxides, and the insertion/removal of each A + in the cathode is accompanied by the concomitant reduction/oxidation of a transition metal ion to accommodate the compensating insertion/removal of an electron. Graphitic carbon is the most common anode.The performance of a rechargeable alkali-ion battery depends crucially on the ease with which alkali ions move in the host crystal of the cathode and anode, in the electrolyte, and in the electrodeelectrolyte interface. Poor alkali transport in any part of the battery

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A high-throughput infrastructure for density functional theory calculations

Cited by 958 publications

References 86 publications

Ligand-Field-Dependent Behavior of Meta-GGA Exchange in Transition-Metal Complex Spin-State Ordering

Ligand-Field-Dependent Behavior of Meta-GGA Exchange in Transition-Metal Complex Spin-State Ordering

Assessing the Thermoelectric Properties of Sintered Compounds via High-ThroughputAb-InitioCalculations

Computational studies of solid-state alkali conduction in rechargeable alkali-ion batteries

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