Intrinsic stoichiometry and oxygen-induced p-type conductivity of pyrite FeS2
The stoichiometry and ubiquitous observation of p-type conductivity of synthetic pyrite FeS[subscript 2] thin films are investigated via first-principles computations of native (vacancies, interstitials, antisites) and extrinsic (O[subscript S], O[subscript i]) point defects. Native defects have hig...
| Main Authors: | , , , |
|---|---|
| Other Authors: | |
| Format: | Article |
| Language: | en_US |
| Published: |
American Physical Society
2011
|
| Online Access: | http://hdl.handle.net/1721.1/67315 https://orcid.org/0000-0002-6833-3480 https://orcid.org/0000-0003-0333-6565 |
| _version_ | 1811080730325811200 |
|---|---|
| author | Sun, Ruoshi Chan, Maria K. Kang, ShinYoung Ceder, Gerbrand |
| author2 | Massachusetts Institute of Technology. Department of Materials Science and Engineering |
| author_facet | Massachusetts Institute of Technology. Department of Materials Science and Engineering Sun, Ruoshi Chan, Maria K. Kang, ShinYoung Ceder, Gerbrand |
| author_sort | Sun, Ruoshi |
| collection | MIT |
| description | The stoichiometry and ubiquitous observation of p-type conductivity of synthetic pyrite FeS[subscript 2] thin films are investigated via first-principles computations of native (vacancies, interstitials, antisites) and extrinsic (O[subscript S], O[subscript i]) point defects. Native defects have high formation energies and are predicted to occur in low concentrations within the Fe- and S-rich limits, showing that pyrite should be intrinsically stoichiometric. Under sufficiently oxidizing conditions, O[subscript S] becomes the most dominant defect type and induces p-type conductivity. At the experimental oxygen impurity concentration, the hole concentration is predicted to be O(10[superscript 19]) cm[superscript −3], in agreement with Hall measurements reported in the literature. Therefore, we attribute the unintentional p-type conductivity of pyrite to oxygen impurities and propose that improvements in device performance may be achieved under more reducing conditions. |
| first_indexed | 2024-09-23T11:35:51Z |
| format | Article |
| id | mit-1721.1/67315 |
| institution | Massachusetts Institute of Technology |
| language | en_US |
| last_indexed | 2024-09-23T11:35:51Z |
| publishDate | 2011 |
| publisher | American Physical Society |
| record_format | dspace |
| spelling | mit-1721.1/673152022-09-27T20:36:18Z Intrinsic stoichiometry and oxygen-induced p-type conductivity of pyrite FeS2 Sun, Ruoshi Chan, Maria K. Kang, ShinYoung Ceder, Gerbrand Massachusetts Institute of Technology. Department of Materials Science and Engineering Ceder, Gerbrand Sun, Ruoshi Chan, Maria K. Kang, ShinYoung Ceder, Gerbrand The stoichiometry and ubiquitous observation of p-type conductivity of synthetic pyrite FeS[subscript 2] thin films are investigated via first-principles computations of native (vacancies, interstitials, antisites) and extrinsic (O[subscript S], O[subscript i]) point defects. Native defects have high formation energies and are predicted to occur in low concentrations within the Fe- and S-rich limits, showing that pyrite should be intrinsically stoichiometric. Under sufficiently oxidizing conditions, O[subscript S] becomes the most dominant defect type and induces p-type conductivity. At the experimental oxygen impurity concentration, the hole concentration is predicted to be O(10[superscript 19]) cm[superscript −3], in agreement with Hall measurements reported in the literature. Therefore, we attribute the unintentional p-type conductivity of pyrite to oxygen impurities and propose that improvements in device performance may be achieved under more reducing conditions. National Science Foundation (U.S.) (Grant No. TG-DMR970008S) 2011-11-30T18:00:09Z 2011-11-30T18:00:09Z 2011-07 2011-05 Article http://purl.org/eprint/type/JournalArticle 1098-0121 1550-235X http://hdl.handle.net/1721.1/67315 Sun, Ruoshi et al. “Intrinsic stoichiometry and oxygen-induced p-type conductivity of pyrite FeS_{2}.” Physical Review B 84 (2011): n. pag. Web. 30 Nov. 2011. © 2011 American Physical Society https://orcid.org/0000-0002-6833-3480 https://orcid.org/0000-0003-0333-6565 en_US http://dx.doi.org/10.1103/PhysRevB.84.035212 Physical Review B Article is made available in accordance with the publisher's policy and may be subject to US copyright law. Please refer to the publisher's site for terms of use. application/pdf American Physical Society APS |
| spellingShingle | Sun, Ruoshi Chan, Maria K. Kang, ShinYoung Ceder, Gerbrand Intrinsic stoichiometry and oxygen-induced p-type conductivity of pyrite FeS2 |
| title | Intrinsic stoichiometry and oxygen-induced p-type conductivity of pyrite FeS2 |
| title_full | Intrinsic stoichiometry and oxygen-induced p-type conductivity of pyrite FeS2 |
| title_fullStr | Intrinsic stoichiometry and oxygen-induced p-type conductivity of pyrite FeS2 |
| title_full_unstemmed | Intrinsic stoichiometry and oxygen-induced p-type conductivity of pyrite FeS2 |
| title_short | Intrinsic stoichiometry and oxygen-induced p-type conductivity of pyrite FeS2 |
| title_sort | intrinsic stoichiometry and oxygen induced p type conductivity of pyrite fes2 |
| url | http://hdl.handle.net/1721.1/67315 https://orcid.org/0000-0002-6833-3480 https://orcid.org/0000-0003-0333-6565 |
| work_keys_str_mv | AT sunruoshi intrinsicstoichiometryandoxygeninducedptypeconductivityofpyritefes2 AT chanmariak intrinsicstoichiometryandoxygeninducedptypeconductivityofpyritefes2 AT kangshinyoung intrinsicstoichiometryandoxygeninducedptypeconductivityofpyritefes2 AT cedergerbrand intrinsicstoichiometryandoxygeninducedptypeconductivityofpyritefes2 |