Rational design of transparent p-type conducting non-oxide materials from high-throughput calculations

Raghupathy, Ramya Kormath Madam; Kühne, Thomas D.; Felser, Claudia; Mirhosseini, Hossein

doi:10.1039/c7tc05311h

Cited by 29 publications

(33 citation statements)

References 69 publications

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“…• p-type dopability: Gauge whether a material should be intrinsically p-type dopable or suffers from significant compensation using calculations of various complexity, from bulk structure branch point energies (BPEs) 47,49 to more expensive intrinsic/extrinsic defect calculations. 44,54 • Refinements: Tailor the output set from the preceding calculations to specific areas of interest, e.g. surface slab calculations to estimate band alignment, 52 electrochemical stability, further refinements on optical prop-4 erties, materials availability and toxicity considerations, 2D materials calculations to compare bulk structures with monolayers, 54 etc.…”

Section: Introductionmentioning

confidence: 99%

“…44,54 • Refinements: Tailor the output set from the preceding calculations to specific areas of interest, e.g. surface slab calculations to estimate band alignment, 52 electrochemical stability, further refinements on optical prop-4 erties, materials availability and toxicity considerations, 2D materials calculations to compare bulk structures with monolayers, 54 etc.…”

Section: Introductionmentioning

confidence: 99%

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Assessing High-Throughput Descriptors for Prediction of Transparent Conductors

Woods‐Robinson

Broberg²,

Faghaninia

et al. 2018

Chem. Mater.

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The growth of materials databases has yielded significant quantities of data to mine for new energy materials using high-throughput screening methodologies. One application of interest to energy and optoelectronics is the prediction of new high performing p-type transparent conductors (TCs). However, screening methods for such materials have never been validated over the breadth of computed materials properties. In this study, we compile an experimental data set of 74 bulk crystal structures corresponding to known state-of-the-art n-type and p-type TCs, and compute a series of corresponding computational descriptor properties. Our goals are to (1) compare computational descriptors to experimentally demonstrated properties of real materials in the data set, (2) determine the ability of ground state, density functional theory (DFT)-based computational screening methodologies to identify these experimentally realized TCs, and 1 (3) use this understanding to estimate reasonable screening cutoffs for four commonly used descriptors. First, stability calculations demonstrate that most materials in the data set have an energy above the convex hull (E hull) of less than 100 meV/atom, and we also propose a Pourbaix analysis technique to estimate moisture stability. Second, we find a lenient cutoff for the DFT PBE band gap of 0.5 eV is sufficient to include a majority of the wide gap candidates and exclude narrow gap compounds. Next, the effective mass, m * , is found to correlate weakly to conductivity in the p-type materials as compared with n-type materials, which may motivate an increase in the m * cutoff as well. Lastly, we perform an uncertainty analysis and literature comparison for the branch point energy (BPE), a qualitative descriptor for dopability. We find the BPEs of most n-type materials to lie near the conduction band and those of most p-type materials to lie at mid-gap; this is a significant distinction, suggesting BPE to be a more definitive descriptor for n-type TC materials. By assessing the validity of this simple screening methodology via comparing experimental data to computational descriptors, we aim to motivate and strengthen future materials discovery efforts in the field of transparent conductors and beyond.

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Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Assessing High-Throughput Descriptors for Prediction of Transparent Conductors

Woods‐Robinson

Broberg²,

Faghaninia

et al. 2018

Chem. Mater.

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“…16 Another material class identified is binary nonoxide compounds. 15,18 These materials possess a VBM with significant contributions from anion p-states, which for nonoxide anions are more delocalized than the 2p orbitals of oxygen. 18 Materials such as sulfides, iodides, and especially phosphides 13,15,16,19,22 were found via highthroughput screening and first-principles calculations to commonly have m Ã h < 5 m e , with phosphides including many examples <1 m e , owing to the metal-p and phosphorous-p orbital mixing at the VBM.…”

Section: Computational Screening For Disperse Valence Band Materialsmentioning

confidence: 99%

“…15,18 These materials possess a VBM with significant contributions from anion p-states, which for nonoxide anions are more delocalized than the 2p orbitals of oxygen. 18 Materials such as sulfides, iodides, and especially phosphides 13,15,16,19,22 were found via highthroughput screening and first-principles calculations to commonly have m Ã h < 5 m e , with phosphides including many examples <1 m e , owing to the metal-p and phosphorous-p orbital mixing at the VBM. 15 Notable p-TCM candidates in these material classes are boron phosphide (BP), 15 copper iodide (CuI), [22][23][24] CuAlS 2 , 25,26 (Zr,Hf)OS, 16,27 and Mg:LaCuOSe.…”

Section: Computational Screening For Disperse Valence Band Materialsmentioning

confidence: 99%

“…These predictions are based on coupling dispersion (delocalization) of the valence band (VB) with favorable defect formation chemistry in order to select materials with inherently high hole mobility and enhanced p-type dopability. [15][16][17][18] However, experimental realization of these materials currently lags behind theoretical predictions, creating an evident gap between computationally predicted disperse valence band materials (DVMs) and their experimental investigation. In this review, we present an overview of the experimental techniques and synthesis approaches reported on DVMs with the aim to bridge the gap between computational and experimental works on p-TCMs.…”

Section: Introductionmentioning

confidence: 99%

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Bridging the p-type transparent conductive materials gap: synthesis approaches for disperse valence band materials

Fioretti

Morales‐Masis

2020

J. Photon. Energy

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Transparent conductive materials (TCMs) with high p-type conductivity and broadband transparency have remained elusive for years. Despite decades of research, no p-type material has yet been found to match the performance of n-type TCMs. If developed, the high-performance p-type TCMs would lead to significant advances in a wide range of technologies, including thin-film transistors, transparent electronics, flat screen displays, and photovoltaics. Recent insights from high-throughput computational screening have defined design principles for identifying candidate materials with low hole effective mass, also known as disperse valence band materials. Particularly, materials with mixed-anion chemistry and nonoxide materials have received attention as being promising next-generation p-type TCMs. However, experimental demonstrations of these compounds are scarce compared to the computational output. One reason for this gap is the experimental difficulty of safely and controllably sourcing elements, such as sulfur, phosphorous, and iodine for depositing these materials in thin-film form. Another important obstacle to experimental realization is air stability or stability with respect to formation of the competing oxide phases. We summarize experimental demonstrations of disperse valence band materials, including synthesis strategies and common experimental challenges. We end by outlining recommendations for synthesizing p-type TCMs still absent from the literature and highlight remaining experimental barriers to be overcome.

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Wide‐Range‐Tunable p‐Type Conductivity of Transparent CuI₁₋_xBr_x Alloy

Yamada

Tanida

Murata

et al. 2020

Adv Funct Materials

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Transparent p-type semiconductors with wide-range tunability of the hole density are rare. Developing such materials is a challenge in the field of transparent electronics that utilize invisible electric circuits. In this paper, a CuI-CuBr alloy (CuI 1−x Br x ) is proposed as a hole-density-tunable p-type transparent semiconductor that can be fabricated at room temperature. First-principles calculations predict that the acceptor state originating from copper vacancies in CuBr is deeper than that in CuI, leading to the hypothesis that the hole density in CuI 1−x Br x can be tuned over a wide range by varying x between 0 and 1. The experimental results support this hypothesis. The hole density in CuI 1−x Br x polycrystalline alloy layers can be tuned by over three orders of magnitude (10 17 -10 20 cm −3 ) by varying x. In other words, the p-type conductivity of the CuI 1−x Br x alloy shows metallic and semiconducting properties. Such alloy layers can be prepared at room temperature without sacrificing transparency. Furthermore, CuI 1−x Br x forms transparent p-n diodes with n-type amorphous In-Ga-Zn-O layers, and these diodes have satisfactory rectification performance. Therefore, CuI 1−x Br x alloy is an excellent p-type transparent semiconductor for which the p-type conductivity can be tailored in a wide range.

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Rational design of transparent p-type conducting non-oxide materials from high-throughput calculations

Abstract: In this work, high-throughput ab initio calculations are employed to identify the most promising chalcogenide-based semiconductors for p-type transparent conducting materials (TCMs).

Cited by 29 publications

References 69 publications

Assessing High-Throughput Descriptors for Prediction of Transparent Conductors

Assessing High-Throughput Descriptors for Prediction of Transparent Conductors

Bridging the p-type transparent conductive materials gap: synthesis approaches for disperse valence band materials

Wide‐Range‐Tunable p‐Type Conductivity of Transparent CuI₁₋_xBr_x Alloy

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Rational design of transparent p-type conducting non-oxide materials from high-throughput calculations

Abstract: In this work, high-throughput ab initio calculations are employed to identify the most promising chalcogenide-based semiconductors for p-type transparent conducting materials (TCMs).

Cited by 29 publications

References 69 publications

Assessing High-Throughput Descriptors for Prediction of Transparent Conductors

Assessing High-Throughput Descriptors for Prediction of Transparent Conductors

Bridging the p-type transparent conductive materials gap: synthesis approaches for disperse valence band materials

Wide‐Range‐Tunable p‐Type Conductivity of Transparent CuI1−xBrx Alloy

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Wide‐Range‐Tunable p‐Type Conductivity of Transparent CuI₁₋_xBr_x Alloy