A New Three-Dimensional Subsulfide Ir2In8S with Dirac Semimetal Behavior

Khoury, Jason F.; Rettie, Alexander J.  E.; Khan, Mojammel A.; Ghimire, Nirmal J.; Robredo, Iñigo; Pfluger, Jonathan E.; Pal, Koushik; Wolverton, Chris; Bergara, Aitor; Jiang, J. S.; Schoop, Leslie M.; Vergniory, Maia G.; Mitchell, J. F.; Chung, Duck Young; Kanatzidis, Mercouri G.

doi:10.1021/jacs.9b10147

Title: A New Three-Dimensional Subsulfide Ir₂In₈S with Dirac Semimetal Behavior

Abstract

Dirac and Weyl semimetals host exotic quasiparticles with unconventional transport properties, such as high magnetoresistance and carrier mobility. Recent years have witnessed a huge number of newly predicted topological semimetals from existing databases; however, experimental verification often lags behind such predictions. Common reasons are synthetic difficulties or the stability of predicted phases. Here, we report the synthesis of the type-II Dirac semimetal Ir2In8S, an air-stable compound with a new structure type. This material has two Dirac crossings in its electronic structure along the Γ-Z direction of the Brillouin zone. We further show that Ir2In8S has a high electron carrier mobility of ~10 000 cm2/(V s) at 1.8 K and a large, nonsaturating transverse magnetoresistance of ~6000% at 3.34 K in a 14 T applied field. Shubnikov de-Haas oscillations reveal several small Fermi pockets and the possibility of a nontrivial Berry phase. With its facile crystal growth, novel structure type, and striking electronic structure, Ir2In8S introduces a new material system to study topological semimetals and enable advances in the field of topological materials.

Authors:

^[1];

^[2]; Khan, Mojammel A. ^[3]; Ghimire, Nirmal J. ^[4]; Robredo, Iñigo ^[5]; Pfluger, Jonathan E. ^[1]; Pal, Koushik ^[1];

^[1]; Bergara, Aitor ^[6]; Jiang, J. S. ^[3];

^[7]; Vergniory, Maia G. ^[8]; Mitchell, J. F. ^[3]; Chung, Duck Young ^[3];

^[9]

Northwestern Univ., Evanston, IL (United States)
Argonne National Lab. (ANL), Argonne, IL (United States); Univ. College London, Bloomsbury (United Kingdom)
Argonne National Lab. (ANL), Argonne, IL (United States)
Argonne National Lab. (ANL), Argonne, IL (United States); George Mason Univ., Fairfax, VA (United States)
Donostia International Physics Center (Spain); Univ. of the Basque Country, Donostia (Spain)
Donostia International Physics Center (Spain); Univ. of the Basque Country, Donostia (Spain); Centro Mixto CSIC-UPV/EHU, Donostia (Spain)
Princeton Univ., NJ (United States)
Donostia International Physics Center (Spain)n; Ikerbasque Basque Foundation for Science (Spain)
Northwestern Univ., Evanston, IL (United States); Argonne National Lab. (ANL), Argonne, IL (United States)

Publication Date:: Thu Nov 07 00:00:00 EST 2019

Research Org.:: Argonne National Laboratory (ANL), Argonne, IL (United States); Northwestern Univ., Evanston, IL (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division; National Science Foundation (NSF)

OSTI Identifier:: 1581283

Alternate Identifier(s):: OSTI ID: 1776865

Grant/Contract Number:: AC02-06CH11357; SC0014520; DMR-1420541; DMR-1708254

Resource Type:: Accepted Manuscript

Journal Name:: Journal of the American Chemical Society

Additional Journal Information:: Journal Volume: 141; Journal Issue: 48; Journal ID: ISSN 0002-7863

Publisher:: American Chemical Society (ACS)

Country of Publication:: United States

Language:: English

Subject:: 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats


                    Khoury, Jason F., Rettie, Alexander J.  E., Khan, Mojammel A., Ghimire, Nirmal J., Robredo, Iñigo, Pfluger, Jonathan E., Pal, Koushik, Wolverton, Chris, Bergara, Aitor, Jiang, J. S., Schoop, Leslie M., Vergniory, Maia G., Mitchell, J. F., Chung, Duck Young, and Kanatzidis, Mercouri G. A New Three-Dimensional Subsulfide Ir2In8S with Dirac Semimetal Behavior.  United States: N. p., 2019. 
Web.  doi:10.1021/jacs.9b10147.

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                    Khoury, Jason F., Rettie, Alexander J.  E., Khan, Mojammel A., Ghimire, Nirmal J., Robredo, Iñigo, Pfluger, Jonathan E., Pal, Koushik, Wolverton, Chris, Bergara, Aitor, Jiang, J. S., Schoop, Leslie M., Vergniory, Maia G., Mitchell, J. F., Chung, Duck Young, & Kanatzidis, Mercouri G. A New Three-Dimensional Subsulfide Ir2In8S with Dirac Semimetal Behavior.  United States.  https://doi.org/10.1021/jacs.9b10147

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                    Khoury, Jason F., Rettie, Alexander J.  E., Khan, Mojammel A., Ghimire, Nirmal J., Robredo, Iñigo, Pfluger, Jonathan E., Pal, Koushik, Wolverton, Chris, Bergara, Aitor, Jiang, J. S., Schoop, Leslie M., Vergniory, Maia G., Mitchell, J. F., Chung, Duck Young, and Kanatzidis, Mercouri G. Thu .  
"A New Three-Dimensional Subsulfide Ir2In8S with Dirac Semimetal Behavior".  United States.  https://doi.org/10.1021/jacs.9b10147.  https://www.osti.gov/servlets/purl/1581283.

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@article{osti_1581283,

  title        = {A New Three-Dimensional Subsulfide Ir2In8S with Dirac Semimetal Behavior},

  author       = {Khoury, Jason F. and Rettie, Alexander J.  E. and Khan, Mojammel A. and Ghimire, Nirmal J. and Robredo, Iñigo and Pfluger, Jonathan E. and Pal, Koushik and Wolverton, Chris and Bergara, Aitor and Jiang, J. S. and Schoop, Leslie M. and Vergniory, Maia G. and Mitchell, J. F. and Chung, Duck Young and Kanatzidis, Mercouri G.},

  abstractNote = {Dirac and Weyl semimetals host exotic quasiparticles with unconventional transport properties, such as high magnetoresistance and carrier mobility. Recent years have witnessed a huge number of newly predicted topological semimetals from existing databases; however, experimental verification often lags behind such predictions. Common reasons are synthetic difficulties or the stability of predicted phases. Here, we report the synthesis of the type-II Dirac semimetal Ir2In8S, an air-stable compound with a new structure type. This material has two Dirac crossings in its electronic structure along the Γ-Z direction of the Brillouin zone. We further show that Ir2In8S has a high electron carrier mobility of ~10 000 cm2/(V s) at 1.8 K and a large, nonsaturating transverse magnetoresistance of ~6000% at 3.34 K in a 14 T applied field. Shubnikov de-Haas oscillations reveal several small Fermi pockets and the possibility of a nontrivial Berry phase. With its facile crystal growth, novel structure type, and striking electronic structure, Ir2In8S introduces a new material system to study topological semimetals and enable advances in the field of topological materials.},

  doi          = {10.1021/jacs.9b10147},

  journal      = {Journal of the American Chemical Society},

  number       = 48,

  volume       = 141,

  place        = {United States},

  year         = {Thu Nov 07 00:00:00 EST 2019},

  month        = {Thu Nov 07 00:00:00 EST 2019}

}

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Title: A New Three-Dimensional Subsulfide Ir2In8S with Dirac Semimetal Behavior

Abstract

Citation Formats

A stable three-dimensional topological Dirac semimetal Cd3As2 journal, May 2014

Transport evidence for Fermi-arc-mediated chirality transfer in the Dirac semimetal Cd3As2 journal, July 2016

Ultrahigh mobility and giant magnetoresistance in the Dirac semimetal Cd3As2 journal, November 2014

Discovery of a Three-Dimensional Topological Dirac Semimetal, Na3Bi journal, January 2014

Experimental Realization of a Three-Dimensional Dirac Semimetal journal, July 2014

Chemical Principles of Topological Semimetals journal, April 2018

Topological semimetals predicted from first-principles calculations journal, June 2016

Tunable Weyl and Dirac states in the nonsymmorphic compound CeSbTe journal, February 2018

Extremely large magnetoresistance and ultrahigh mobility in the topological Weyl semimetal candidate NbP journal, June 2015

Ferromagnetic ordering and half-metallic state of Sn 2 Co 3 S 2 with the shandite-type structure journal, October 2013

Giant anomalous Hall effect in a ferromagnetic kagome-lattice semimetal journal, July 2018

Large intrinsic anomalous Hall effect in half-metallic ferromagnet Co3Sn2S2 with magnetic Weyl fermions journal, September 2018

Observation of the Chiral-Anomaly-Induced Negative Magnetoresistance in 3D Weyl Semimetal TaAs journal, August 2015

Directly photoexcited Dirac and Weyl fermions in ZrSiS and NbAs journal, November 2018

Two-dimensional type-II Dirac fermions in layered oxides journal, August 2018

Band Structure Perfection and Superconductivity in Type‐II Dirac Semimetal Ir 1− x Pt x Te 2 journal, July 2018

Topological Superconductivity in Dirac Semimetals journal, October 2015

Lorentz-violating type-II Dirac fermions in transition metal dichalcogenide PtTe2 journal, August 2017

Quantum oscillations and a nontrivial Berry phase in the noncentrosymmetric topological superconductor candidate BiPd journal, January 2019

Nontrivial Berry phase and type-II Dirac transport in the layered material PdT e 2 journal, July 2017

Experimental Realization of Type-II Dirac Fermions in a PdTe 2 Superconductor journal, July 2017

Beware of plausible predictions of fantasy materials journal, February 2019

Topological Semimetals in Square-Net Materials journal, July 2019

Triple Point Topological Metals journal, July 2016

Topological semimetals with triply degenerate nodal points in θ -phase tantalum nitride journal, June 2016

Comprehensive search for topological materials using symmetry indicators journal, February 2019

Catalogue of topological electronic materials journal, February 2019

A complete catalogue of high-quality topological materials journal, February 2019

A New Magnetic Topological Quantum Material Candidate by Design journal, April 2019

Topology Shapes a Search for New Materials journal, May 2018

Stacked topological insulator built from bismuth-based graphene sheet analogues journal, March 2013

Charge-density-wave superconductor Bi 2 Rh 3 Se 2 journal, February 2007

Transport properties in normal-metal Bi 2 Pd 3 S 2 and superconducting Bi 2 Pd 3 Se 2 journal, July 2008

Use of frit-disc crucibles for routine and exploratory solution growth of single crystalline samples journal, December 2015

Development of viable solutions for the synthesis of sulfur bearing single crystals journal, July 2012

New Metal-Rich Sulfides Ni6SnS2 and Ni9Sn2S2 with a 2D Metal Framework: Synthesis, Crystal Structure, and Bonding journal, September 2003

Unique Metallic Wires in a Novel Quasi-1D Compound. Synthesis, Crystal and Electronic Structure, and Properties of Ni 8 Bi 8 SI journal, December 2001

Preparation and crystal structure of Nb14S5 journal, March 1973

The crystal structure of Zr9S2 journal, May 1972

Structure and bonding in metal-rich compounds: Pnictides, chalcides and halides journal, January 1978

Bi5,6Ni5I: Eine partiell oxidierte intermetallische Phase mit Kanalstruktur journal, December 1995

From the Metal to the Molecule—Ternary Bismuth Subhalides journal, April 2001

At the edge of covalency: metallic nanotubes, low-dimensional metals and clusters journal, January 2010

The PseudoDojo: Training and grading a 85 element optimized norm-conserving pseudopotential table journal, May 2018

Advanced capabilities for materials modelling with Quantum ESPRESSO journal, October 2017

QUANTUM ESPRESSO: a modular and open-source software project for quantum simulations of materials journal, September 2009

Tilted anisotropic Dirac cones in quinoid-type graphene and α − ( BEDT-TTF ) 2 I 3 journal, July 2008

π Berry phase and Zeeman splitting of Weyl semimetal TaP journal, January 2016

Correlation of crystal quality and extreme magnetoresistance of WTe 2 journal, June 2015

Large, non-saturating magnetoresistance in WTe2 journal, September 2014

Compensated Semimetal LaSb with Unsaturated Magnetoresistance journal, September 2016

Large magnetoresistance in compensated semimetals TaAs 2 and NbAs 2 journal, May 2016

Magnetic Oscillations in Metals book, October 2011

Self-Consistent Equations Including Exchange and Correlation Effects journal, November 1965

Inhomogeneous Electron Gas journal, November 1964

Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set journal, October 1996

From ultrasoft pseudopotentials to the projector augmented-wave method journal, January 1999

Generalized Gradient Approximation Made Simple journal, October 1996

Fully unconstrained noncollinear magnetism within the projector augmented-wave method journal, November 2000

Anisotropic angular magnetoresistance and Fermi surface topology of the candidate novel topological metal Pd 3 Pb journal, August 2018

IrRep: Symmetry eigenvalues and irreducible representations of ab initio band structures text, January 2022

Title: A New Three-Dimensional Subsulfide Ir₂In₈S with Dirac Semimetal Behavior

A stable three-dimensional topological Dirac semimetal Cd3As2
journal, May 2014

Transport evidence for Fermi-arc-mediated chirality transfer in the Dirac semimetal Cd3As2
journal, July 2016

Ultrahigh mobility and giant magnetoresistance in the Dirac semimetal Cd3As2
journal, November 2014

Discovery of a Three-Dimensional Topological Dirac Semimetal, Na3Bi
journal, January 2014

Experimental Realization of a Three-Dimensional Dirac Semimetal
journal, July 2014

Chemical Principles of Topological Semimetals
journal, April 2018

Topological semimetals predicted from first-principles calculations
journal, June 2016

Tunable Weyl and Dirac states in the nonsymmorphic compound CeSbTe
journal, February 2018

Extremely large magnetoresistance and ultrahigh mobility in the topological Weyl semimetal candidate NbP
journal, June 2015

Ferromagnetic ordering and half-metallic state of Sn $_{2}$ Co $_{3}$ S $_{2}$ with the shandite-type structure
journal, October 2013

Giant anomalous Hall effect in a ferromagnetic kagome-lattice semimetal
journal, July 2018

Large intrinsic anomalous Hall effect in half-metallic ferromagnet Co3Sn2S2 with magnetic Weyl fermions
journal, September 2018

Observation of the Chiral-Anomaly-Induced Negative Magnetoresistance in 3D Weyl Semimetal TaAs
journal, August 2015

Directly photoexcited Dirac and Weyl fermions in ZrSiS and NbAs
journal, November 2018

Two-dimensional type-II Dirac fermions in layered oxides
journal, August 2018

Band Structure Perfection and Superconductivity in Type‐II Dirac Semimetal Ir ₁₋ _x Pt _x Te ₂
journal, July 2018

Topological Superconductivity in Dirac Semimetals
journal, October 2015

Lorentz-violating type-II Dirac fermions in transition metal dichalcogenide PtTe2
journal, August 2017

Quantum oscillations and a nontrivial Berry phase in the noncentrosymmetric topological superconductor candidate BiPd
journal, January 2019

Nontrivial Berry phase and type-II Dirac transport in the layered material $PdT e_{2}$
journal, July 2017

Experimental Realization of Type-II Dirac Fermions in a ${PdTe}_{2}$ Superconductor
journal, July 2017

Beware of plausible predictions of fantasy materials
journal, February 2019

Topological Semimetals in Square-Net Materials
journal, July 2019

Triple Point Topological Metals
journal, July 2016

Topological semimetals with triply degenerate nodal points in $θ$ -phase tantalum nitride
journal, June 2016

Comprehensive search for topological materials using symmetry indicators
journal, February 2019

Catalogue of topological electronic materials
journal, February 2019

A complete catalogue of high-quality topological materials
journal, February 2019

A New Magnetic Topological Quantum Material Candidate by Design
journal, April 2019

Topology Shapes a Search for New Materials
journal, May 2018

Stacked topological insulator built from bismuth-based graphene sheet analogues
journal, March 2013

Charge-density-wave superconductor ${Bi}_{2} {Rh}_{3} {Se}_{2}$
journal, February 2007

Transport properties in normal-metal ${Bi}_{2} {Pd}_{3} S_{2}$ and superconducting ${Bi}_{2} {Pd}_{3} {Se}_{2}$
journal, July 2008

Use of frit-disc crucibles for routine and exploratory solution growth of single crystalline samples
journal, December 2015

Development of viable solutions for the synthesis of sulfur bearing single crystals
journal, July 2012

New Metal-Rich Sulfides Ni₆SnS₂ and Ni₉Sn₂S₂ with a 2D Metal Framework: Synthesis, Crystal Structure, and Bonding
journal, September 2003

Unique Metallic Wires in a Novel Quasi-1D Compound. Synthesis, Crystal and Electronic Structure, and Properties of Ni ₈ Bi ₈ SI
journal, December 2001

Preparation and crystal structure of Nb14S5
journal, March 1973

The crystal structure of Zr9S2
journal, May 1972

Structure and bonding in metal-rich compounds: Pnictides, chalcides and halides
journal, January 1978

Bi5,6Ni5I: Eine partiell oxidierte intermetallische Phase mit Kanalstruktur
journal, December 1995

From the Metal to the Molecule—Ternary Bismuth Subhalides
journal, April 2001

At the edge of covalency: metallic nanotubes, low-dimensional metals and clusters
journal, January 2010

The PseudoDojo: Training and grading a 85 element optimized norm-conserving pseudopotential table
journal, May 2018

Advanced capabilities for materials modelling with Quantum ESPRESSO
journal, October 2017

QUANTUM ESPRESSO: a modular and open-source software project for quantum simulations of materials
journal, September 2009

Tilted anisotropic Dirac cones in quinoid-type graphene and $α − {(BEDT-TTF)}_{2} I_{3}$
journal, July 2008

π Berry phase and Zeeman splitting of Weyl semimetal TaP
journal, January 2016

Correlation of crystal quality and extreme magnetoresistance of WTe ₂
journal, June 2015

Large, non-saturating magnetoresistance in WTe2
journal, September 2014

Compensated Semimetal LaSb with Unsaturated Magnetoresistance
journal, September 2016

Large magnetoresistance in compensated semimetals ${TaAs}_{2}$ and ${NbAs}_{2}$
journal, May 2016

Magnetic Oscillations in Metals
book, October 2011

Self-Consistent Equations Including Exchange and Correlation Effects
journal, November 1965

Inhomogeneous Electron Gas
journal, November 1964

Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set
journal, October 1996

From ultrasoft pseudopotentials to the projector augmented-wave method
journal, January 1999

Generalized Gradient Approximation Made Simple
journal, October 1996

Fully unconstrained noncollinear magnetism within the projector augmented-wave method
journal, November 2000

Anisotropic angular magnetoresistance and Fermi surface topology of the candidate novel topological metal ${Pd}_{3} Pb$
journal, August 2018

IrRep: Symmetry eigenvalues and irreducible representations of ab initio band structures
text, January 2022