The Subchalcogenides Ir2In8Q (Q = S, Se, Te): Dirac Semimetal Candidates with Re-entrant Structural Modulation

Khoury, Jason F.; Rettie, Alexander J.  E.; Robredo, Iñigo; Krogstad, Matthew J.; Malliakas, Christos D.; Bergara, Aitor; Vergniory, Maia G.; Osborn, Raymond; Rosenkranz, Stephan; Chung, Duck Young; Kanatzidis, Mercouri G.

doi:10.1021/jacs.0c00809

Title: The Subchalcogenides Ir₂In₈Q (Q = S, Se, Te): Dirac Semimetal Candidates with Re-entrant Structural Modulation

Journal Article · Wed Mar 11 00:00:00 EDT 2020 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.0c00809· OSTI ID:1631579

^[1];

^[2]; Robredo, Iñigo ^[3]; Krogstad, Matthew J. ^[4];

^[1]; Bergara, Aitor ^[3]; Vergniory, Maia G. ^[5]; Osborn, Raymond ^[4];

^[4]; Chung, Duck Young ^[4];

^[6]

Northwestern Univ., Evanston, IL (United States). Dept. of Chemistry
Argonne National Lab. (ANL), Argonne, IL (United States). Materials Science Division; Univ. College London (United Kingdom)
Donostia International Physics Center (Spain); Univ. of the Basque Country, Bilbao (Spain). Condensed Matter Physics Dept.
Argonne National Lab. (ANL), Argonne, IL (United States). Materials Science Division
Univ. of the Basque Country, Bilbao (Spain). Condensed Matter Physics Dept.
Northwestern Univ., Evanston, IL (United States). Dept. of Chemistry; Argonne National Lab. (ANL), Argonne, IL (United States). Materials Science Division

Subchalcogenides are uncommon compounds where the metal atoms are in unusually low formal oxidation states. They bridge the gap between intermetallics and semiconductors and can have unexpected structures and properties because of the exotic nature of their chemical bonding as they contain both metal–metal and metal–main group (e.g., halide, chalcogenide) interactions. Finding new members of this class of materials presents synthetic challenges as attempts to make them often result in phase separation into binary compounds. We overcome this difficulty by utilizing indium as a metal flux to synthesize large (millimeter scale) single crystals of novel subchalcogenide materials. Herein, we report two new compounds Ir₂In₈Q (Q = Se, Te) and compare their structural and electrical properties to the previously reported Ir₂In₈S analogue. Ir₂In₈Se and Ir₂In₈Te crystallize in the $$P_{4_2}$$/mnm space group and are isostructural to Ir2In8S, but also have commensurately modulated (with q vectors q = 1/6a* + 1/6b* and q = 1/10a* + 1/10b* for Ir₂In₈Se and Ir₂In₈Te, respectively) low-temperature phase transitions, where the chalcogenide anions in the channels experience a distortion in the form of In–Q bond alternation along the ab plane. Both compounds display re-entrant structural behavior, where the supercells appear on cooling but revert to the original subcell below 100 K, suggesting competing structural and electronic interactions dictate the overall structure. Notably, these materials are topological semimetal candidates with symmetry-protected Dirac crossings near the Fermi level and exhibit high electron mobilities (~1500 cm² V^–1 s^–1 at 1.8 K) and moderate carrier concentrations (~10²⁰ cm^–3) from charge transport measurements. This work highlights metal flux as a synthetic route to high quality single crystals of novel intermetallic subchalcogenides with Dirac semimetal behavior.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division; USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division

Contributing Organization:: State of Illinois; Northwestern University - International Institute for Nanotechnology (IIN); Spanish Ministerio de Economia y Competitividad (MINECO)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1631579

Journal Information:: Journal of the American Chemical Society, Vol. 142, Issue 13; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 6 works

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CSD 1979252: Experimental Crystal Structure Determination F., Khoury, Jason; E., Rettie, Alexander J.; Iñigo, Robredo, https://doi.org/10.25505/fiz.icsd.cc24fkv0 The current record is supplemented by this dataset	dataset	January 2020
CSD 1979253: Experimental Crystal Structure Determination F., Khoury, Jason; E., Rettie, Alexander J.; Iñigo, Robredo, https://doi.org/10.25505/fiz.icsd.cc24fkw1 The current record is supplemented by this dataset	dataset	January 2020
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Title: The Subchalcogenides Ir2In8Q (Q = S, Se, Te): Dirac Semimetal Candidates with Re-entrant Structural Modulation

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