Local orbital degeneracy lifting as a precursor to an orbital-selective Peierls transition

Bozin, Emil S.; Yin, W. G.; Koch, R. J.; Abeykoon, M.; Hor, Y. S.; Zheng, H.; Lei, H. C.; Petrovic, C.; Mitchell, J. F.; Billinge, S. J.  L.

doi:10.1038/s41467-019-11372-w

Title: Local orbital degeneracy lifting as a precursor to an orbital-selective Peierls transition

Abstract

Fundamental electronic principles underlying all transition metal compounds are the symmetry and filling of the d-electron orbitals and the influence of this filling on structural configurations and responses. Here we use a sensitive local structural technique, x-ray atomic pair distribution function analysis, to reveal the presence of fluctuating local-structural distortions at high temperature in one such compound, CuIr₂S₄. We show that this hitherto overlooked fluctuating symmetry-lowering is electronic in origin and will modify the energy-level spectrum and electronic and magnetic properties. The explanation is a local, fluctuating, orbital-degeneracy-lifted state. The natural extension of our result would be that this phenomenon is likely to be widespread amongst diverse classes of partially filled nominally degenerate d-electron systems, with potentially broad implications for our understanding of their properties.

Authors:

^[1];

^[1]; Koch, R. J. ^[1]; Abeykoon, M. ^[1]; Hor, Y. S. ^[2]; Zheng, H. ^[2]; Lei, H. C. ^[1]; Petrovic, C. ^[1]; Mitchell, J. F. ^[2];

^[3]

Brookhaven National Lab. (BNL), Upton, NY (United States)
Argonne National Lab. (ANL), Argonne, IL (United States)
Brookhaven National Lab. (BNL), Upton, NY (United States); Columbia Univ., New York, NY (United States)

Publication Date:: 2019-08-13

Research Org.:: Argonne National Laboratory (ANL), Argonne, IL (United States); Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)

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

OSTI Identifier:: 1560035

Alternate Identifier(s):: OSTI ID: 1543404; OSTI ID: 1670676

Report Number(s):: BNL-211872-2019-JAAM; BNL-219937-2020-JAAM
Journal ID: ISSN 2041-1723; 150997

Grant/Contract Number:: AC02-06CH11357; SC0012704

Resource Type:: Accepted Manuscript

Journal Name:: Nature Communications

Additional Journal Information:: Journal Volume: 10; Journal Issue: 1; Journal ID: ISSN 2041-1723

Publisher:: Nature Publishing Group

Country of Publication:: United States

Language:: English

Subject:: 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; 36 MATERIALS SCIENCE; Electronic properties and materials; Structure of solids and liquids

Citation Formats


                    Bozin, Emil S., Yin, W. G., Koch, R. J., Abeykoon, M., Hor, Y. S., Zheng, H., Lei, H. C., Petrovic, C., Mitchell, J. F., and Billinge, S. J.  L.. Local orbital degeneracy lifting as a precursor to an orbital-selective Peierls transition.  United States: N. p., 2019. 
Web.  doi:10.1038/s41467-019-11372-w.

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                    Bozin, Emil S., Yin, W. G., Koch, R. J., Abeykoon, M., Hor, Y. S., Zheng, H., Lei, H. C., Petrovic, C., Mitchell, J. F., & Billinge, S. J.  L.. Local orbital degeneracy lifting as a precursor to an orbital-selective Peierls transition.  United States.  https://doi.org/10.1038/s41467-019-11372-w

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                    Bozin, Emil S., Yin, W. G., Koch, R. J., Abeykoon, M., Hor, Y. S., Zheng, H., Lei, H. C., Petrovic, C., Mitchell, J. F., and Billinge, S. J.  L.. Tue .  
"Local orbital degeneracy lifting as a precursor to an orbital-selective Peierls transition".  United States.  https://doi.org/10.1038/s41467-019-11372-w.  https://www.osti.gov/servlets/purl/1560035.

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@article{osti_1560035,

  title        = {Local orbital degeneracy lifting as a precursor to an orbital-selective Peierls transition},

  author       = {Bozin, Emil S. and Yin, W. G. and Koch, R. J. and Abeykoon, M. and Hor, Y. S. and Zheng, H. and Lei, H. C. and Petrovic, C. and Mitchell, J. F. and Billinge, S. J.  L.},

  abstractNote = {Fundamental electronic principles underlying all transition metal compounds are the symmetry and filling of the d-electron orbitals and the influence of this filling on structural configurations and responses. Here we use a sensitive local structural technique, x-ray atomic pair distribution function analysis, to reveal the presence of fluctuating local-structural distortions at high temperature in one such compound, CuIr2S4. We show that this hitherto overlooked fluctuating symmetry-lowering is electronic in origin and will modify the energy-level spectrum and electronic and magnetic properties. The explanation is a local, fluctuating, orbital-degeneracy-lifted state. The natural extension of our result would be that this phenomenon is likely to be widespread amongst diverse classes of partially filled nominally degenerate d-electron systems, with potentially broad implications for our understanding of their properties.},

  doi          = {10.1038/s41467-019-11372-w},

  journal      = {Nature Communications},

  number       = 1,

  volume       = 10,

  place        = {United States},

  year         = {2019},

  month        = {8}

}

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Fig. 1: Observation of high-temperature fluctuating ODL state in CuIr₂S₄. a Temperature waterfall stack of xPDFs measured on warming from 10 K (bottom) to 500 K (top) in 2 K increments. T_MI is the MIT transition temperature (226 K). The dimer peak at ~3 Å (marked by arrow) is onlymore »

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Works referencing / citing this record:

Slow dynamics of disordered zigzag chain molecules in layered LiVS2 under electron irradiation
text, January 2021

Katayama, Naoyuki; Kojima, Keita; Yamaguchi, Tomoki
arXiv
DOI: 10.48550/arxiv.2102.09795

Nanoscale degeneracy lifting in a geometrically frustrated antiferromagnet
text, January 2020

Frandsen, Benjamin A.; Bozin, Emil S.; Aza, Eleni
arXiv
DOI: 10.48550/arxiv.2001.09917

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Fig. 1 (p. 5)

Fig. 2 (p. 6)

Fig. 3 (p. 7)

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Title: Local orbital degeneracy lifting as a precursor to an orbital-selective Peierls transition

Abstract

Citation Formats

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Imaging Orbital-selective Quasiparticles in the Hund's Metal State of FeSe text, January 2018

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Covalent bonds against magnetism in transition metal compounds text, January 2016

Effect of magnetic frustration on nematicity and superconductivity in Fe chalcogenides text, January 2015

Pressure Induced Metal-Insulator Transition of Selenospinel CuIr 2 Se 4 journal, May 1997

Orbital symmetry of charge-density-wave order in La1.875Ba0.125CuO4 and YBa2Cu3O6.67 journal, February 2016

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Formation of isomorphic Ir3+ and Ir4+ octamers and spin dimerization in the spinel CuIr2S4
journal, March 2002

Room temperature local nematicity in FeSe superconductor
journal, July 2019

Photoinduced dynamics of nematic order parameter in FeSe
journal, May 2019

Hopping Conductivity in CuIr ₂ S ₄ Spinel Compound: I. Empirical Model for Electronic Configuration and Mechanism of Metal–Insulator Transition
journal, July 2006

Pseudogap and charge density waves in two dimensions
text, January 2007

Imaging Orbital-selective Quasiparticles in the Hund's Metal State of FeSe
text, January 2018

Spin Ice State in Frustrated Magnetic Pyrochlore Materials
journal, November 2001

Widespread orthorhombic fluctuations in the $(Sr, Na) {Fe}_{2} {As}_{2}$ family of superconductors
journal, November 2018

Effect of magnetic frustration on nematicity and superconductivity in iron chalcogenides
journal, August 2015

PDFgetX3 : a rapid and highly automatable program for processing powder diffraction data into total scattering pair distribution functions
journal, March 2013

Fermi surface nesting and the origin of charge density waves in metals
journal, April 2008

Discovery of Orbital-Selective Cooper Pairing in FeSe
text, January 2016

Fermi Surface Nesting and Nanoscale Fluctuating Charge/Orbital Ordering in Colossal Magnetoresistive Oxides
journal, April 2001

Photoemission study of the metal-insulator transition in ${CuIr}_{2}$ $S_{4}$
journal, June 1997

Structural, magnetic, and electrical properties of Li $_{2}$ Ir $_{1 - x}$ Ru $_{x}$ O $_{3}$
journal, January 2014

Lattice effects in magnetoresistive manganese perovskites
journal, March 1998

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

Orthogonal Magnetization and Symmetry Breaking in Pyrochlore Iridate Eu2Ir2O7
text, January 2016

X-Ray Photoemission Study of ${CuIr}_{2} S_{4} : {Ir}^{3 +} − {Ir}^{4 +}$ Charge Ordering and the Effect of Light Illumination
journal, December 2005

Anomalous resistivity and thermopower of the spinel-type compounds ${CuIr}_{2} S_{4}$ and ${CuIr}_{2} {Se}_{4}$
journal, April 2000

Orbital-driven nematicity in FeSe
journal, November 2014

Control of the metal–insulator transition in vanadium dioxide by modifying orbital occupancy
journal, September 2013

Jahn-Teller distortion driven magnetic polarons in magnetite
journal, June 2017

Orbital molecules in electronic materials
journal, April 2015

Orbital symmetry of charge-density-wave order in La1.875Ba0.125CuO4 and YBa2Cu3O6.67
journal, February 2016

Detailed Mapping of the Local ${Ir}^{4 +}$ Dimers through the Metal-Insulator Transitions of ${CuIr}_{2} S_{4}$ Thiospinel by X-Ray Atomic Pair Distribution Function Measurements
journal, January 2011

Nematicity and quantum paramagnetism in FeSe
journal, September 2015

In-gap state and effect of light illumination in ${CuIr}_{2} S_{4}$ probed by photoemission spectroscopy
journal, December 2008

From quantum matter to high-temperature superconductivity in copper oxides
journal, February 2015

Nematicity and quantum paramagnetism in FeSe
journal, September 2015

Electronic nematicity above the structural and superconducting transition in BaFe2(As1−xP x )2
journal, June 2012

Frustration-induced nanometre-scale inhomogeneity in a triangular antiferromagnet
journal, January 2014

Cu(Ir1 − xCrx)2S4: a model system for studying nanoscale phase coexistence at the metal-insulator transition
journal, February 2014

Bilayer manganites reveal polarons in the midst of a metallic breakdown
journal, September 2011

Imaging orbital-selective quasiparticles in the Hund’s metal state of FeSe
journal, September 2018

Orbital ordering in transition-metal spinels
journal, January 2005

Lattice effects in magnetoresistive manganese perovskites
journal, March 1998

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

Observation of Orbital Currents in CuO
journal, April 2011

Covalent bonds against magnetism in transition metal compounds
journal, September 2016

Metal-insulator transition in ${CuIr}_{2} S_{4} :$ XAS results on the electronic structure
journal, May 2003

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

Rapidly fluctuating orbital occupancy above the orbital ordering transition in spin-gap compounds
text, January 2010

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

Formation of isomorphic Ir3+ and Ir4+ octamers and spin dimerization in the spinel CuIr2S4
journal, March 2002

Fermi Surface Nesting and Nanoscale Fluctuating Charge/Orbital Ordering in Colossal Magnetoresistive Oxides
text, January 2001

Metal-insulator transition in the spinel-type ${CuIr}_{2} (S_{1 - x} {Se}_{x})_{4}$ system
journal, September 1998

Direct Observation of Lattice Polaron Formation in the Local Structure of ${La}_{1 - x} {Ca}_{x} {MnO}_{3}$
journal, July 1996

Pseudogap and Charge Density Waves in Two Dimensions
journal, May 2008

Orbital selectivity enhanced by nematic order in FeSe
text, January 2018

Bending and breaking of stripes in a charge ordered manganite
journal, December 2017

Gap Opening and Orbital Modification of Superconducting FeSe above the Structural Distortion
journal, June 2012

Pseudogap and charge density waves in two dimensions
text, January 2007

Orbital molecules in electronic materials
journal, April 2015

Orbital-driven nematicity in FeSe
journal, November 2014

Frustration-induced nanometre-scale inhomogeneity in a triangular antiferromagnet
journal, January 2014

Phase-Sensitive Observation of a Spin-Orbital Mott State in Sr2IrO4
journal, March 2009

Orbital Correlations in the Pseudocubic $O$ and Rhombohedral $R$ Phases of ${LaMnO}_{3}$
journal, May 2005

Orbital symmetry of charge density wave order in La1.875Ba0.125CuO4 and YBa2Cu3O6.67
text, January 2014

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

Gap opening and orbital modification of superconducting FeSe above the structural distortion
text, January 2012

Orbitally Induced Peierls State in Spinels
journal, April 2005

Imaging Orbital-selective Quasiparticles in the Hund's Metal State of FeSe
text, January 2018

Fluctuation Effects at a Peierls Transition
journal, August 1973

Covalent bonds against magnetism in transition metal compounds
text, January 2016

Effect of magnetic frustration on nematicity and superconductivity in Fe chalcogenides
text, January 2015

Pressure Induced Metal-Insulator Transition of Selenospinel CuIr ₂ Se ₄
journal, May 1997

Orbital symmetry of charge-density-wave order in La1.875Ba0.125CuO4 and YBa2Cu3O6.67
journal, February 2016

Opposite pressure effects in the orbitally-induced Peierls phase transition systems CuIr ₂ S ₄ and MgTi ₂ O ₄
journal, January 2017

Origin of band gaps in 3d perovskite oxides
text, January 2019

Suppression of metal-to-insulator transition and appearance of superconductivity in ${Cu}_{1 - x} {Zn}_{x} {Ir}_{2} S_{4}$
journal, November 2001

Fermi surface nesting induced strong pairing in iron-based superconductors
text, January 2008

Polaron freezing and the quantum liquid-crystal phase in the ferromagnetic metallic La0.67Ca0.33MnO3
journal, April 2018

Selective Mott Physics as a Key to Iron Superconductors
journal, April 2014

Rapid-acquisition pair distribution function (RA-PDF) analysis
journal, November 2003

Structural compliance, misfit strain and stripe nanostructures in cuprate superconductors
text, January 2001

Fermi surface nesting induced strong pairing in iron-based superconductors
journal, April 2009

Fermi surface nesting induced strong pairing in iron-based superconductors
text, January 2008

Structural compliance, misfit strain, and stripe nanostructures in cuprate superconductors
journal, August 2002

Observation of Orbital Currents in CuO
journal, April 2011