Evolution of structure and magnetism across the metal-insulator transition in the pyrochlore iridate (Nd1–xCax)2Ir2O7

Porter, Zach; Zoghlin, Eli; Britner, Samuel; Husremovic, Samra; Ruff, Jacob P.C.; Choi, Yongseong; Haskel, Daniel; Laurita, Geneva; Wilson, Stephen D.

doi:10.1103/PhysRevB.100.054409

Title: Evolution of structure and magnetism across the metal-insulator transition in the pyrochlore iridate ${({Nd}_{1 - x} {Ca}_{x})}_{2} {Ir}_{2} O_{7}$

Abstract

We report on the evolution of the thermal metal-insulator transition in polycrystalline samples of Nd₂Ir₂O₇ upon hole doping via substitution of Ca²⁺ for Nd³⁺. Ca substitution mediates a filling-controlled Mott-like transition with minimal resolvable structural changes and without altering site symmetry. Local structure confirms that Ca substitution does not result in local chemical phase separation, and absorption spectroscopy establishes that Ir cations maintain a spin-orbit entangled electronic configuration. The metal-insulator transition coincides with antiferromagnetic ordering on the Ir sublattice for all measured samples, and both decrease in onset temperature with Ca content. As a result, weak low-temperature upturns in susceptibility and resistivity for samples with high Ca content suggest that Nd sublattice antiferromagnetism continues to couple to carriers in the metallic regime.

Authors:

Porter, Zach ^[1]; Zoghlin, Eli ^[1]; Britner, Samuel ^[2]; Husremovic, Samra ^[2]; Ruff, Jacob P.C. ^[3]; Choi, Yongseong ^[4]; Haskel, Daniel ^[4];

^[2]; Wilson, Stephen D. ^[1]

Univ. of California, Santa Barbara, CA (United States)
Bates College, Lewiston, ME (United States)
Cornell Univ., Ithaca, NY (United States)
Argonne National Lab. (ANL), Argonne, IL (United States)

Publication Date:: Thu Aug 08 00:00:00 EDT 2019

Research Org.:: Argonne National Lab. (ANL), Argonne, IL (United States)

Sponsoring Org.:: US Army Research Office (ARO); National Science Foundation (NSF); USDOE Office of Science (SC)

OSTI Identifier:: 1577100

Alternate Identifier(s):: OSTI ID: 1550583

Grant/Contract Number:: AC02-06CH11357

Resource Type:: Accepted Manuscript

Journal Name:: Physical Review B

Additional Journal Information:: Journal Volume: 100; Journal Issue: 5; Journal ID: ISSN 2469-9950

Publisher:: American Physical Society (APS)

Country of Publication:: United States

Language:: English

Subject:: 36 MATERIALS SCIENCE

Citation Formats


                    Porter, Zach, Zoghlin, Eli, Britner, Samuel, Husremovic, Samra, Ruff, Jacob P.C., Choi, Yongseong, Haskel, Daniel, Laurita, Geneva, and Wilson, Stephen D. Evolution of structure and magnetism across the metal-insulator transition in the pyrochlore iridate (Nd1–xCax)2Ir2O7.  United States: N. p., 2019. 
Web.  doi:10.1103/PhysRevB.100.054409.

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                    Porter, Zach, Zoghlin, Eli, Britner, Samuel, Husremovic, Samra, Ruff, Jacob P.C., Choi, Yongseong, Haskel, Daniel, Laurita, Geneva, & Wilson, Stephen D. Evolution of structure and magnetism across the metal-insulator transition in the pyrochlore iridate (Nd1–xCax)2Ir2O7.  United States.  https://doi.org/10.1103/PhysRevB.100.054409

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                    Porter, Zach, Zoghlin, Eli, Britner, Samuel, Husremovic, Samra, Ruff, Jacob P.C., Choi, Yongseong, Haskel, Daniel, Laurita, Geneva, and Wilson, Stephen D. Thu .  
"Evolution of structure and magnetism across the metal-insulator transition in the pyrochlore iridate (Nd1–xCax)2Ir2O7".  United States.  https://doi.org/10.1103/PhysRevB.100.054409.  https://www.osti.gov/servlets/purl/1577100.

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@article{osti_1577100,

  title        = {Evolution of structure and magnetism across the metal-insulator transition in the pyrochlore iridate (Nd1–xCax)2Ir2O7},

  author       = {Porter, Zach and Zoghlin, Eli and Britner, Samuel and Husremovic, Samra and Ruff, Jacob P.C. and Choi, Yongseong and Haskel, Daniel and Laurita, Geneva and Wilson, Stephen D.},

  abstractNote = {We report on the evolution of the thermal metal-insulator transition in polycrystalline samples of Nd2Ir2O7 upon hole doping via substitution of Ca2+ for Nd3+. Ca substitution mediates a filling-controlled Mott-like transition with minimal resolvable structural changes and without altering site symmetry. Local structure confirms that Ca substitution does not result in local chemical phase separation, and absorption spectroscopy establishes that Ir cations maintain a spin-orbit entangled electronic configuration. The metal-insulator transition coincides with antiferromagnetic ordering on the Ir sublattice for all measured samples, and both decrease in onset temperature with Ca content. As a result, weak low-temperature upturns in susceptibility and resistivity for samples with high Ca content suggest that Nd sublattice antiferromagnetism continues to couple to carriers in the metallic regime.},

  doi          = {10.1103/PhysRevB.100.054409},

  journal      = {Physical Review B},

  number       = 5,

  volume       = 100,

  place        = {United States},

  year         = {Thu Aug 08 00:00:00 EDT 2019},

  month        = {Thu Aug 08 00:00:00 EDT 2019}

}

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https://doi.org/10.1103/PhysRevB.100.054409

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Cited by: 7 works

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Figures / Tables:

FIG. 1: Synchrotron XRD patterns in circles, all taken at 300 K. Calculated curves include the pyrochlore phase and the impurity phases Ir, IrO₂, and Nd₂O₃. Lines above the residual curves index only pyrochlore peaks.

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Title: Evolution of structure and magnetism across the metal-insulator transition in the pyrochlore iridate ( Nd 1 – x Ca x ) 2 Ir 2 O 7

Abstract

Citation Formats

Figures / Tables:

Comparative study of low-temperature x-ray diffraction experiments on R 2 Ir 2 O 7 ( R = Nd , Eu, and Pr) journal, December 2014

Coulombic Quantum Liquids in Spin- 1 / 2 Pyrochlores journal, January 2012

Magnetization and Hall effect studies on the pyrochlore iridate Nd 2 Ir 2 O 7 journal, February 2013

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Robust pinning of magnetic moments in pyrochlore iridates journal, September 2017

Topological and magnetic phases of interacting electrons in the pyrochlore iridates journal, January 2012

Variation of Charge Dynamics in the Course of Metal-Insulator Transition for Pyrochlore-Type Nd 2 Ir 2 O 7 journal, September 2012

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Odd-parity magnetoresistance in pyrochlore iridate thin films with broken time-reversal symmetry journal, May 2015

Similarities and Differences in the Structural and Electronic Properties of Ruthenium and Iridium PyrochloresA2M2O7−y(M=Ru, Ir) journal, March 1998

Time-reversal symmetry breaking and spontaneous Hall effect without magnetic dipole order journal, December 2009

Metallic Spin-Liquid Behavior of the Geometrically Frustrated Kondo Lattice Pr 2 Ir 2 O 7 journal, March 2006

Magnetic Field-Induced Insulator-Semimetal Transition in a Pyrochlore Nd 2 Ir 2 O 7 journal, July 2015

Spontaneous Hall effect in the Weyl semimetal candidate of all-in all-out pyrochlore iridate journal, August 2018

Slater to Mott Crossover in the Metal to Insulator Transition of Nd 2 Ir 2 O 7 journal, July 2016

Longer-range lattice anisotropy strongly competing with spin-orbit interactions in pyrochlore iridates journal, March 2014

PDFfit2 and PDFgui: computer programs for studying nanostructure in crystals journal, July 2007

Magnetic order in the pyrochlore iridate Nd 2 Ir 2 O 7 probed by muon spin relaxation journal, August 2013

Kitaev-Heisenberg models for iridates on the triangular, hyperkagome, kagome, fcc, and pyrochlore lattices journal, January 2014

Metal–Insulator Transitions in Pyrochlore Oxides Ln 2 Ir 2 O 7 journal, September 2011

Crystal growth and structure of R2Ir2O7 (R=Pr, Eu) using molten KF journal, May 2007

Orbital Magnetism and Spin-Orbit Effects in the Electronic Structure of BaIrO 3 journal, November 2010

Optical evidence for a Weyl semimetal state in pyrochlore Eu 2 Ir 2 O 7 journal, December 2015

Pressure and magnetic field effects on metal-insulator transitions of bulk and domain wall states in pyrochlore iridates journal, September 2015

Magnetic order and the electronic ground state in the pyrochlore iridate Nd 2 Ir 2 O 7 journal, May 2012

PDFgetX2: a GUI-driven program to obtain the pair distribution function from X-ray powder diffraction data journal, July 2004

Dilute magnetism and spin-orbital percolation effects in Sr 2 Ir 1 − x Rh x O 4 journal, February 2014

Bi 2– x Ca x Ir 2 O 6+ y Pyrochlore Phases: Structure and Properties with Varied Ir Oxidation State from 3.9+ to 4.3+ journal, April 2017

Anomalous domain-wall conductance in pyrochlore-type Nd 2 Ir 2 O 7 on the verge of the metal-insulator transition journal, February 2014

X-ray circular dichroism as a probe of orbital magnetization journal, March 1992

Observation of non-Fermi liquid behavior in hole-doped Eu 2 Ir 2 O 7 journal, December 2017

Field-induced quantum metal–insulator transition in the pyrochlore iridate Nd2Ir2O7 journal, November 2015

Pressure Tuning of the Spin-Orbit Coupled Ground State in Sr 2 IrO 4 journal, July 2012

Instrument for x-ray magnetic circular dichroism measurements at high pressures journal, August 2007

Variation of optical conductivity spectra in the course of bandwidth-controlled metal-insulator transitions in pyrochlore iridates journal, June 2016

Mobile metallic domain walls in an all-in-all-out magnetic insulator journal, October 2015

Topological semimetal and Fermi-arc surface states in the electronic structure of pyrochlore iridates journal, May 2011

Two-dimensional detector software: From real detector to idealised image or two-theta scan journal, January 1996

Metal–Insulator Transition in Pyrochlore Iridates Ln 2 Ir 2 O 7 ( Ln = Nd, Sm, and Eu) journal, April 2007

Spin-Orbit Coupling in Iridium-Based 5d Compounds Probed by X-ray Absorption Spectroscopy text, January 2012

Correlated quantum phenomena in the strong spin-orbit regime text, January 2013

A New Type of Quantum Criticality in the Pyrochlore Iridates text, January 2014

Enhanced weak ferromagnetism and conductivity in hole-doped pyrochlore iridate Y2Ir2O7 text, January 2015

Phase diagram of pyrochlore iridates: all-in-all-out magnetic ordering and non-Fermi liquid properties text, January 2015

Pressure and magnetic-field effects on metal-insulator transitions of bulk and domain-wall states in pyrochlore iridates text, January 2015

Robust pinning of magnetic moments in pyrochlore iridates text, January 2017

Dilute stuffing in the pyrochlore iridate $Eu_2Ir_2O_7$ text, January 2018

Title: Evolution of structure and magnetism across the metal-insulator transition in the pyrochlore iridate ${({Nd}_{1 - x} {Ca}_{x})}_{2} {Ir}_{2} O_{7}$

Comparative study of low-temperature x-ray diffraction experiments on $R_{2} {Ir}_{2} O_{7}$ ( $R = Nd$ , Eu, and Pr)
journal, December 2014

Coulombic Quantum Liquids in Spin- $1 / 2$ Pyrochlores
journal, January 2012

Magnetization and Hall effect studies on the pyrochlore iridate Nd $_{2}$ Ir $_{2}$ O $_{7}$
journal, February 2013

Magnetic pyrochlore oxides
journal, January 2010

Dilute stuffing in the pyrochlore iridate ${Eu}_{2} {Ir}_{2} O_{7}$
journal, June 2018

Robust pinning of magnetic moments in pyrochlore iridates
journal, September 2017

Topological and magnetic phases of interacting electrons in the pyrochlore iridates
journal, January 2012

Variation of Charge Dynamics in the Course of Metal-Insulator Transition for Pyrochlore-Type ${Nd}_{2} {Ir}_{2} O_{7}$
journal, September 2012

Iridates from the molecular side
journal, July 2016

Spin-orbit coupling in iridium-based 5 $d$ compounds probed by x-ray absorption spectroscopy
journal, November 2012

Novel $J_{eff} = 1 / 2$ Mott State Induced by Relativistic Spin-Orbit Coupling in ${Sr}_{2} {IrO}_{4}$
journal, August 2008

Correlated Quantum Phenomena in the Strong Spin-Orbit Regime
journal, March 2014

Phase Diagram of Pyrochlore Iridates: All-in–All-out Magnetic Ordering and Non-Fermi-Liquid Properties
journal, October 2015

Enhanced weak ferromagnetism and conductivity in hole-doped pyrochlore iridate $Y_{2} {Ir}_{2} O_{7}$
journal, August 2014

Enhanced thermopower in the correlated semimetallic phase of hole-doped pyrochlore iridates
journal, April 2019

Odd-parity magnetoresistance in pyrochlore iridate thin films with broken time-reversal symmetry
journal, May 2015

Similarities and Differences in the Structural and Electronic Properties of Ruthenium and Iridium PyrochloresA2M2O7−y(M=Ru, Ir)
journal, March 1998

Time-reversal symmetry breaking and spontaneous Hall effect without magnetic dipole order
journal, December 2009

Metallic Spin-Liquid Behavior of the Geometrically Frustrated Kondo Lattice $\Pr_{2} {Ir}_{2} O_{7}$
journal, March 2006

Magnetic Field-Induced Insulator-Semimetal Transition in a Pyrochlore ${Nd}_{2} {Ir}_{2} O_{7}$
journal, July 2015

Spontaneous Hall effect in the Weyl semimetal candidate of all-in all-out pyrochlore iridate
journal, August 2018

Slater to Mott Crossover in the Metal to Insulator Transition of ${Nd}_{2} {Ir}_{2} O_{7}$
journal, July 2016

Longer-range lattice anisotropy strongly competing with spin-orbit interactions in pyrochlore iridates
journal, March 2014

PDFfit2 and PDFgui: computer programs for studying nanostructure in crystals
journal, July 2007

Magnetic order in the pyrochlore iridate Nd $_{2}$ Ir $_{2}$ O $_{7}$ probed by muon spin relaxation
journal, August 2013

Kitaev-Heisenberg models for iridates on the triangular, hyperkagome, kagome, fcc, and pyrochlore lattices
journal, January 2014

Metal–Insulator Transitions in Pyrochlore Oxides Ln ₂ Ir ₂ O ₇
journal, September 2011

Crystal growth and structure of R2Ir2O7 (R=Pr, Eu) using molten KF
journal, May 2007

Orbital Magnetism and Spin-Orbit Effects in the Electronic Structure of ${BaIrO}_{3}$
journal, November 2010

Optical evidence for a Weyl semimetal state in pyrochlore ${Eu}_{2} {Ir}_{2} O_{7}$
journal, December 2015

Pressure and magnetic field effects on metal-insulator transitions of bulk and domain wall states in pyrochlore iridates
journal, September 2015

Magnetic order and the electronic ground state in the pyrochlore iridate Nd $_{2}$ Ir $_{2}$ O $_{7}$
journal, May 2012

PDFgetX2: a GUI-driven program to obtain the pair distribution function from X-ray powder diffraction data
journal, July 2004

Dilute magnetism and spin-orbital percolation effects in ${Sr}_{2}$ ${Ir}_{1 - x}$ ${Rh}_{x}$ $O_{4}$
journal, February 2014

Bi _{2– x} Ca _x Ir ₂ O _{6+ y} Pyrochlore Phases: Structure and Properties with Varied Ir Oxidation State from 3.9+ to 4.3+
journal, April 2017

Anomalous domain-wall conductance in pyrochlore-type ${Nd}_{2} {Ir}_{2} O_{7}$ on the verge of the metal-insulator transition
journal, February 2014

X-ray circular dichroism as a probe of orbital magnetization
journal, March 1992

Observation of non-Fermi liquid behavior in hole-doped ${Eu}_{2} {Ir}_{2} O_{7}$
journal, December 2017

Field-induced quantum metal–insulator transition in the pyrochlore iridate Nd2Ir2O7
journal, November 2015

Pressure Tuning of the Spin-Orbit Coupled Ground State in ${Sr}_{2} {IrO}_{4}$
journal, July 2012

Instrument for x-ray magnetic circular dichroism measurements at high pressures
journal, August 2007

Variation of optical conductivity spectra in the course of bandwidth-controlled metal-insulator transitions in pyrochlore iridates
journal, June 2016

Mobile metallic domain walls in an all-in-all-out magnetic insulator
journal, October 2015

Topological semimetal and Fermi-arc surface states in the electronic structure of pyrochlore iridates
journal, May 2011

Two-dimensional detector software: From real detector to idealised image or two-theta scan
journal, January 1996

Metal–Insulator Transition in Pyrochlore Iridates Ln ₂ Ir ₂ O ₇ ( Ln = Nd, Sm, and Eu)
journal, April 2007

Spin-Orbit Coupling in Iridium-Based 5d Compounds Probed by X-ray Absorption Spectroscopy
text, January 2012

Correlated quantum phenomena in the strong spin-orbit regime
text, January 2013

A New Type of Quantum Criticality in the Pyrochlore Iridates
text, January 2014

Enhanced weak ferromagnetism and conductivity in hole-doped pyrochlore iridate Y2Ir2O7
text, January 2015

Phase diagram of pyrochlore iridates: all-in-all-out magnetic ordering and non-Fermi liquid properties
text, January 2015

Pressure and magnetic-field effects on metal-insulator transitions of bulk and domain-wall states in pyrochlore iridates
text, January 2015

Robust pinning of magnetic moments in pyrochlore iridates
text, January 2017

Dilute stuffing in the pyrochlore iridate $Eu_2Ir_2O_7$
text, January 2018