Structural Tolerance Factor Approach to Defect-Resistant I<inf>2</inf>-II-IV-X<inf>4</inf> Semiconductor Design
dc.contributor.author | Sun, JP | |
dc.contributor.author | McKeown Wessler, GC | |
dc.contributor.author | Wang, T | |
dc.contributor.author | Zhu, T | |
dc.contributor.author | Blum, V | |
dc.contributor.author | Mitzi, DB | |
dc.date.accessioned | 2020-10-15T19:05:44Z | |
dc.date.available | 2020-10-15T19:05:44Z | |
dc.date.issued | 2020-02-25 | |
dc.date.updated | 2020-10-15T19:05:22Z | |
dc.description.abstract | Copyright © 2020 American Chemical Society. Recent work on quaternary semiconductors Cu2BaSn(S,Se)4 and Ag2BaSnSe4 for photovoltaic and thermoelectric applications, respectively, has shown the promise of exploring the broader family of defect-resistant I2-II-IV-X4 materials (where I, II, and IV refer to the formal oxidation state of the metal cations and X is a chalcogen anion) with tetrahedrally coordinated I/IV cations and larger II cations (i.e., Sr, Ba, Pb, and Eu) for optoelectronic and energy-related applications. Chemical dissimilarity among the II and I/IV atoms represents an important design motivation because it presents a barrier to antisite formation, which otherwise may act as electronically harmful defects. We herein show how all 31 experimentally reported I2-II-IV-X4 examples (with large II cations and tetrahedrally coordinated smaller I/IV cations), which form within five crystal structure types, are structurally linked. Based on these structural similarities, we derive a set of tolerance factors that serve as descriptors for phase stability within this family. Despite common usage in the well-studied perovskite system, Shannon ionic radii are found to be insufficient for predicting metal-chalcogen bond lengths, pointing to the need for experimentally derived correction factors as part of an empirically driven learning approach to structure prediction. We use the tolerance factors as a predictive tool and demonstrate that four new I2-II-IV-X4 compounds, Ag2BaSiS4, Ag2PbSiS4, Cu2PbGeS4, and Cu2SrSiS4, can be synthesized in correctly predicted phases. One of these compounds, Ag2PbSiS4, shows potentially promising optoelectronic properties for photovoltaic applications. | |
dc.identifier.issn | 0897-4756 | |
dc.identifier.issn | 1520-5002 | |
dc.identifier.uri | ||
dc.language | en | |
dc.publisher | American Chemical Society (ACS) | |
dc.relation.ispartof | Chemistry of Materials | |
dc.relation.isversionof | 10.1021/acs.chemmater.9b05107 | |
dc.subject | Science & Technology | |
dc.subject | Physical Sciences | |
dc.subject | Technology | |
dc.subject | Chemistry, Physical | |
dc.subject | Materials Science, Multidisciplinary | |
dc.subject | Chemistry | |
dc.subject | Materials Science | |
dc.subject | CRYSTAL-STRUCTURE | |
dc.subject | M-IV | |
dc.subject | INTERATOMIC DISTANCES | |
dc.subject | OPTICAL PERFORMANCES | |
dc.subject | RELATIVE STABILITY | |
dc.subject | HYBRID FUNCTIONALS | |
dc.subject | GE | |
dc.subject | CHALCOGENIDE | |
dc.subject | SN | |
dc.subject | SR | |
dc.title | Structural Tolerance Factor Approach to Defect-Resistant I2-II-IV-X4 Semiconductor Design | |
dc.type | Journal article | |
duke.contributor.orcid | Blum, V|0000-0001-8660-7230 | |
duke.contributor.orcid | Mitzi, DB|0000-0001-5189-4612 | |
pubs.begin-page | 1636 | |
pubs.end-page | 1649 | |
pubs.issue | 4 | |
pubs.organisational-group | Pratt School of Engineering | |
pubs.organisational-group | Chemistry | |
pubs.organisational-group | Mechanical Engineering and Materials Science | |
pubs.organisational-group | Duke | |
pubs.organisational-group | Trinity College of Arts & Sciences | |
pubs.organisational-group | Student | |
pubs.publication-status | Published | |
pubs.volume | 32 |
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