Synthetic control over polymorph formation in the d-band semiconductor system FeS 2
Pyrite, also known as fool's gold is the thermodynamic stable polymorph of FeS 2 . It is widely considered as a promising d-band semiconductor for various applications due to its intriguing physical properties. Marcasite is the other naturally occurring polymorph of FeS 2 . Measurements on natu...
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Published in | Chemical science (Cambridge) Vol. 12; no. 41; pp. 13870 - 13877 |
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Main Authors | , , , , , , |
Format | Journal Article |
Language | English |
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Royal Society of Chemistry (RSC)
27.10.2021
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Abstract | Pyrite, also known as fool's gold is the thermodynamic stable polymorph of FeS
2
. It is widely considered as a promising d-band semiconductor for various applications due to its intriguing physical properties. Marcasite is the other naturally occurring polymorph of FeS
2
. Measurements on natural crystals have shown that it has similarly promising electronic, mechanical, and optical properties as pyrite. However, it has been only scarcely investigated so far, because the laboratory-based synthesis of phase-pure samples or high quality marcasite single crystal has been a challenge until now. Here, we report the targeted phase formation
via
hydrothermal synthesis of marcasite and pyrite. The formation condition and phase purity of the FeS
2
polymorphs are systematically studied in the form of a comprehensive synthesis map. We, furthermore, report on a detailed analysis of marcasite single crystal growth by a space-separated hydrothermal synthesis. We observe that single phase product of marcasite forms only on the surface under the involvement of H
2
S and sulphur vapor. The availability of high-quality crystals of marcasite allows us to measure the fundamental physical properties, including an allowed direct optical bandgap of 0.76 eV, temperature independent diamagnetism, an electronic transport gap of 0.11 eV, and a room-temperature carrier concentration of 4.14 × 10
18
cm
−3
. X-ray absorption/emission spectroscopy are employed to measure the band gap of the two FeS
2
phases. We find marcasite has a band gap of 0.73 eV, while pyrite has a band gap of 0.87 eV. Our results indicate that marcasite – that is now synthetically available in a straightforward fashion – is as equally promising as pyrite as candidate for various semiconductor applications based on earth abundant elements. |
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AbstractList | Pyrite, also known as fool's gold is the thermodynamic stable polymorph of FeS
2
. Pyrite, also known as fool's gold is the thermodynamic stable polymorph of FeS 2 . It is widely considered as a promising d-band semiconductor for various applications due to its intriguing physical properties. Marcasite is the other naturally occurring polymorph of FeS 2 . Measurements on natural crystals have shown that it has similarly promising electronic, mechanical, and optical properties as pyrite. However, it has been only scarcely investigated so far, because the laboratory-based synthesis of phase-pure samples or high quality marcasite single crystal has been a challenge until now. Here, we report the targeted phase formation via hydrothermal synthesis of marcasite and pyrite. The formation condition and phase purity of the FeS 2 polymorphs are systematically studied in the form of a comprehensive synthesis map. We, furthermore, report on a detailed analysis of marcasite single crystal growth by a space-separated hydrothermal synthesis. We observe that single phase product of marcasite forms only on the surface under the involvement of H 2 S and sulphur vapor. The availability of high-quality crystals of marcasite allows us to measure the fundamental physical properties, including an allowed direct optical bandgap of 0.76 eV, temperature independent diamagnetism, an electronic transport gap of 0.11 eV, and a room-temperature carrier concentration of 4.14 × 10 18 cm −3 . X-ray absorption/emission spectroscopy are employed to measure the band gap of the two FeS 2 phases. We find marcasite has a band gap of 0.73 eV, while pyrite has a band gap of 0.87 eV. Our results indicate that marcasite – that is now synthetically available in a straightforward fashion – is as equally promising as pyrite as candidate for various semiconductor applications based on earth abundant elements. |
Author | von Rohr, Fabian O. Lago, Jorge Yang, Wanli Li, Qingtian Lefèvre, Robin Blacque, Olivier Ma, KeYuan |
Author_xml | – sequence: 1 givenname: KeYuan surname: Ma fullname: Ma, KeYuan organization: Department of Chemistry, University of Zurich, CH-8057 Zürich, Switzerland – sequence: 2 givenname: Robin surname: Lefèvre fullname: Lefèvre, Robin organization: Department of Chemistry, University of Zurich, CH-8057 Zürich, Switzerland – sequence: 3 givenname: Qingtian surname: Li fullname: Li, Qingtian organization: Advanced Light Source, Lawrence Berkeley National Laboratory, Berkeley, California 94720, USA, State Key Laboratory of Functional Materials for Informatics, Chinese Academy of Sciences, Shanghai 200050, China, University of Chinese Academy of Sciences, Beijing 100049, China – sequence: 4 givenname: Jorge surname: Lago fullname: Lago, Jorge organization: Department of Chemistry, University of Zurich, CH-8057 Zürich, Switzerland, Department of Inorganic Chemistry, Univ. del Pais Vasco (UPV-EHU), 48080 Bilbao, Spain – sequence: 5 givenname: Olivier orcidid: 0000-0001-9857-4042 surname: Blacque fullname: Blacque, Olivier organization: Department of Chemistry, University of Zurich, CH-8057 Zürich, Switzerland – sequence: 6 givenname: Wanli orcidid: 0000-0003-0666-8063 surname: Yang fullname: Yang, Wanli organization: Advanced Light Source, Lawrence Berkeley National Laboratory, Berkeley, California 94720, USA – sequence: 7 givenname: Fabian O. orcidid: 0000-0003-0422-6042 surname: von Rohr fullname: von Rohr, Fabian O. organization: Department of Chemistry, University of Zurich, CH-8057 Zürich, Switzerland |
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CitedBy_id | crossref_primary_10_1021_acs_chemmater_3c00760 crossref_primary_10_1016_j_electacta_2022_141409 crossref_primary_10_1016_j_seppur_2024_127856 |
Cites_doi | 10.1016/0375-9601(80)90454-5 10.1180/minmag.1993.057.386.02 10.1021/jz301023c 10.1039/C3SC52977K 10.1021/acsnano.6b00065 10.1016/B978-0-444-63303-3.00014-6 10.1039/C8TA06312E 10.1021/acs.accounts.7b00187 10.1021/cr0503658 10.1016/0022-0248(68)90067-5 10.1039/C5CS00151J 10.1016/0927-0248(93)90095-K 10.1021/ar0000105 10.1021/acsnano.5b04700 10.1149/1.2108553 10.1016/0016-7037(91)90050-F 10.1021/jacs.7b07044 10.1021/ja1096368 10.1016/0016-7037(86)90214-0 10.1021/acs.chemmater.5b03562 10.1007/BF02398183 10.1016/j.ssc.2016.01.004 10.1071/CH9960867 10.1016/j.cplett.2004.09.028 10.1016/0038-1098(77)90422-7 10.1039/C8SC03555E 10.1021/acsami.7b00578 10.1021/cm901273v 10.1021/acscatal.5b01637 10.1007/3-540-27946-6_29 10.1103/PhysRevB.83.235311 10.1103/PhysRevB.88.235203 10.2138/am-1996-1-215 10.1021/acs.inorgchem.9b01017 10.1016/0021-9614(76)90135-X 10.1021/acssuschemeng.0c03675 10.1103/PhysRevB.79.035108 10.1021/acs.jpcc.5b11482 10.1039/C7CP04413E 10.1016/j.jallcom.2020.154173 10.1039/C5RA22610D 10.1021/acsmaterialslett.0c00207 10.1038/ncomms13799 |
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Snippet | Pyrite, also known as fool's gold is the thermodynamic stable polymorph of FeS
2
. It is widely considered as a promising d-band semiconductor for various... Pyrite, also known as fool's gold is the thermodynamic stable polymorph of FeS 2 . |
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Title | Synthetic control over polymorph formation in the d-band semiconductor system FeS 2 |
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