Magnetization dynamics fingerprints of an excitonic condensate t2g4 magnet

Kaushal, Nitin; Herbrych, Jacek; Alvarez, Gonzalo; Dagotto, Elbio R.

doi:10.1103/physrevb.104.235135

Title: Magnetization dynamics fingerprints of an excitonic condensate $t_{2 g}^{4}$ magnet

Abstract

The competition between spin-orbit coupling (SOC) $λ$ and electron-electron interaction $U$ leads to a plethora of novel states of matter, extensively studied in the context of $t_{2 g}^{4}$ and $t_{2 g}^{5}$ materials, such as ruthenates and iridates. Excitonic magnets—the antiferromagnetic state of bounded electron-hole pairs-are prominent examples of phenomena driven by those competing energy scales. Interestingly, recent theoretical studies predicted that excitonic magnets can be found in the ground state of SOC $t_{2 g}^{4}$ Hubbard models. Here we present a detailed computational study of the magnetic excitations in that excitonic magnet, employing one-dimensional chains (via density matrix renormalization group) and small two-dimensional clusters (via Lanczos). Specifically, first we show that the low-energy spectrum is dominated by a dispersive (acoustic) magnonic mode, with extra features arising from the $λ = 0$ state in the phase diagram. Second, and more importantly, we found a novel magnetic excitation forming a high-energy optical mode with the highest intensity at wave-vector $q \to 0$ . In the excitonic condensation regime at large $U$ , we also have found a novel high-energy $π$ mode composed solely of orbital excitations. Overall, these features do not appear all together in any of the neighboring states in the phase diagram and thus constitute unique fingerprints of the $t_{2 g}^{4}$ excitonic magnet, of importance in the analysis of neutron and resonant inelastic x-ray scattering experiments.

Authors:

Kaushal, Nitin ^[1]; Herbrych, Jacek ^[2];

^[3]; Dagotto, Elbio R. ^[4]

Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Wroclaw Univ. of Science and Technology (Poland)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)

Publication Date:: Mon Dec 20 00:00:00 EST 2021

Research Org.:: Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division; Polish National Agency for Academic Exchange (NAWA); National Science Centre Poland (NCN)

OSTI Identifier:: 1838948

Grant/Contract Number:: AC05-00OR22725; PPN/PPO/2018/1/00035; 2019/35/B/ST3/01207

Resource Type:: Accepted Manuscript

Journal Name:: Physical Review B

Additional Journal Information:: Journal Volume: 104; Journal Issue: 23; Journal ID: ISSN 2469-9950

Publisher:: American Physical Society (APS)

Country of Publication:: United States

Language:: English

Subject:: 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; magnetism; spin-orbit coupling; antiferromagnets; Bose-Einstein condensates; iridates

Citation Formats


                    Kaushal, Nitin, Herbrych, Jacek, Alvarez, Gonzalo, and Dagotto, Elbio R. Magnetization dynamics fingerprints of an excitonic condensate t2g4 magnet.  United States: N. p., 2021. 
Web.  doi:10.1103/physrevb.104.235135.

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                    Kaushal, Nitin, Herbrych, Jacek, Alvarez, Gonzalo, & Dagotto, Elbio R. Magnetization dynamics fingerprints of an excitonic condensate t2g4 magnet.  United States.  https://doi.org/10.1103/physrevb.104.235135

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                    Kaushal, Nitin, Herbrych, Jacek, Alvarez, Gonzalo, and Dagotto, Elbio R. Mon .  
"Magnetization dynamics fingerprints of an excitonic condensate t2g4 magnet".  United States.  https://doi.org/10.1103/physrevb.104.235135.  https://www.osti.gov/servlets/purl/1838948.

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@article{osti_1838948,

  title        = {Magnetization dynamics fingerprints of an excitonic condensate t2g4 magnet},

  author       = {Kaushal, Nitin and Herbrych, Jacek and Alvarez, Gonzalo and Dagotto, Elbio R.},

  abstractNote = {The competition between spin-orbit coupling (SOC) λ and electron-electron interaction U leads to a plethora of novel states of matter, extensively studied in the context of t2g4 and t2g5 materials, such as ruthenates and iridates. Excitonic magnets—the antiferromagnetic state of bounded electron-hole pairs-are prominent examples of phenomena driven by those competing energy scales. Interestingly, recent theoretical studies predicted that excitonic magnets can be found in the ground state of SOC t2g4 Hubbard models. Here we present a detailed computational study of the magnetic excitations in that excitonic magnet, employing one-dimensional chains (via density matrix renormalization group) and small two-dimensional clusters (via Lanczos). Specifically, first we show that the low-energy spectrum is dominated by a dispersive (acoustic) magnonic mode, with extra features arising from the λ=0 state in the phase diagram. Second, and more importantly, we found a novel magnetic excitation forming a high-energy optical mode with the highest intensity at wave-vector q→0. In the excitonic condensation regime at large U, we also have found a novel high-energy π mode composed solely of orbital excitations. Overall, these features do not appear all together in any of the neighboring states in the phase diagram and thus constitute unique fingerprints of the t2g4 excitonic magnet, of importance in the analysis of neutron and resonant inelastic x-ray scattering experiments.},

  doi          = {10.1103/physrevb.104.235135},

  journal      = {Physical Review B},

  number       = 23,

  volume       = 104,

  place        = {United States},

  year         = {Mon Dec 20 00:00:00 EST 2021},

  month        = {Mon Dec 20 00:00:00 EST 2021}

}

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Abstract

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Interaction-induced topological phase transition and Majorana edge states in low-dimensional orbital-selective Mott insulators journal, May 2021

Suppression of effective spin-orbit coupling by thermal fluctuations in spin-orbit coupled antiferromagnets journal, July 2021

Novel Magnetism of Ir 5 + ( 5 d 4 ) Ions in the Double Perovskite Sr 2 YIrO 6 journal, February 2014

Weakly coupled alternating S = 1 2 chains in the distorted honeycomb lattice compound Na 2 Cu 2 TeO 6 journal, December 2020

Intertwined charge, spin, and pairing orders in doped iron ladders journal, June 2021

Magnetic Excitation Spectra of Sr 2 IrO 4 Probed by Resonant Inelastic X-Ray Scattering: Establishing Links to Cuprate Superconductors journal, April 2012

Strong Coupling Nature of the Excitonic Insulator State in Ta 2 NiSe 5 journal, June 2018

Excitonic condensation in systems of strongly correlated electrons journal, July 2015

Density-matrix algorithms for quantum renormalization groups journal, October 1993

Anisotropic uniaxial pressure response of the Mott insulator Ca 2 RuO 4 journal, November 2013

Excitonic quasiparticles in a spin–orbit Mott insulator journal, July 2014

Structural and Magnetic Properties of the Iridium Double Perovskites Ba 2– x Sr x YIrO 6 journal, October 2015

Spectral functions with the density matrix renormalization group: Krylov-space approach for correction vectors journal, November 2016

Magnetic states of the quasi-one-dimensional iron chalcogenide Ba 2 FeS 3 journal, September 2021

The density matrix renormalization group for strongly correlated electron systems: A generic implementation journal, September 2009

Orbital-selective Peierls phase in the metallic dimerized chain MoOCl 2 journal, August 2021

Fingerprints of an orbital-selective Mott phase in the block magnetic state of BaFe2Se3 ladders journal, June 2019

First-principles study of the low-temperature charge density wave phase in the quasi-one-dimensional Weyl chiral compound ( TaSe 4 ) 2 I journal, May 2020

Excitonic Magnetism in Van Vleck–type d 4 Mott Insulators journal, November 2013

J Freezing and Hund’s Rules in Spin-Orbit-Coupled Multiorbital Hubbard Models journal, February 2017

Unraveling the Nature of Magnetism of the 5 d 4 Double Perovskite Ba 2 YIrO 6 journal, June 2018

Density matrix formulation for quantum renormalization groups journal, November 1992

Spin-orbital entangled excitonic insulator with quadrupole order journal, February 2019

Origin of magnetic moments and presence of spin-orbit singlets in Ba 2 YIrO 6 journal, July 2018

Crystal and magnetic structure of Ca 2 RuO 4 : Magnetoelastic coupling and the metal-insulator transition journal, July 1998

Zero-gap semiconductor to excitonic insulator transition in Ta2NiSe5 journal, February 2017

Possible spin-orbit driven spin-liquid ground state in the double perovskite phase of Ba 3 YIr 2 O 9 journal, October 2013

Signatures of exciton condensation in a transition metal dichalcogenide journal, December 2017

Origin of the Spin-Orbital Liquid State in a Nearly J = 0 Iridate Ba 3 ZnIr 2 O 9 journal, March 2016

Roles of Hund's rule coupling in excitonic density-wave states journal, December 2014

Higgs mode and its decay in a two-dimensional antiferromagnet journal, March 2017

Excitonic magnetism at the intersection of spin-orbit coupling and crystal-field splitting journal, August 2020

Hopping-Induced Ground-State Magnetism in 6 H Perovskite Iridates journal, July 2019

Strongly Enhanced Tunneling at Total Charge Neutrality in Double-Bilayer Graphene- WSe 2 Heterostructures journal, April 2018

Excitonic Insulator journal, June 1967

Magnetic phases for strongly correlated t 2 g 4 electrons on the square lattice: Impact of spin-orbit coupling and crystal field journal, September 2021

The transition to the metallic state journal, February 1961

Spin-Orbit Physics Giving Rise to Novel Phases in Correlated Systems: Iridates and Related Materials journal, March 2016

Observation of heavy spin-orbit excitons propagating in a nonmagnetic background: The case of ( Ba , Sr ) 2 YIrO 6 journal, February 2018

Dynamical correlation functions using the density matrix renormalization group journal, July 1999

Effective magnetic interactions in spin-orbit coupled d 4 Mott insulators journal, January 2017

Influence of structural distortions on the Ir magnetism in Ba2−xSrxYIrO6 double perovskites journal, June 2016

Neutron and ARPES constraints on the couplings of the multiorbital Hubbard model for the iron pnictides journal, September 2010

Novel J eff = 1 / 2 Mott State Induced by Relativistic Spin-Orbit Coupling in Sr 2 IrO 4 journal, August 2008

Magnetic phase transitions in quantum spin-orbital liquids journal, April 2020

Magnetism out of antisite disorder in the J = 0 compound Ba 2 YIrO 6 journal, October 2017

Highly Anisotropic Magnon Dispersion in Ca 2 RuO 4 : Evidence for Strong Spin Orbit Coupling journal, December 2015

Magnetic excitations in a spin-orbit-coupled d 4 Mott insulator on the square lattice journal, July 2014

Novel Magnetic Block States in Low-Dimensional Iron-Based Superconductors journal, July 2019

Density matrix renormalization group study of a three-orbital Hubbard model with spin-orbit coupling in one dimension journal, October 2017

Study of electronic structure and magnetism in d4 double perovskite iridates A2ScIrO6 (A = Ba, Sr) journal, December 2019

Theory of Superconductivity journal, December 1957

Novel magnetic state in d 4 Mott insulators journal, February 2015

Prediction of exotic magnetic states in the alkali-metal quasi-one-dimensional iron selenide compound Na 2 FeSe 2 journal, July 2020

Spin-orbital excitons and their potential condensation in pentavalent iridates journal, January 2019

Evidence for a low-temperature magnetic ground state in double-perovskite iridates with I r 5 + ( 5 d 4 ) ions journal, August 2017

Giant exciton Fano resonance in quasi-one-dimensional Ta 2 NiSe 5 journal, May 2017

Engineering 1D Quantum Stripes from Superlattices of 2D Layered Materials journal, October 2016

Ba 2 YIrO 6 : A cubic double perovskite material with Ir 5 + ions journal, January 2016

Breakdown of J = 0 nonmagnetic state in d 4 iridate double perovskites: A first-principles study journal, September 2015

Emergence of superconductivity in doped multiorbital Hubbard chains journal, May 2020

The challenge of spin–orbit-tuned ground states in iridates: a key issues review journal, February 2018

Mott transition, spin-orbit effects, and magnetism in Ca 2 RuO 4 journal, February 2017

Spin–orbit effects in pentavalent iridates: models and materials journal, August 2021

Bose–Einstein condensation of excitons in bilayer electron systems journal, December 2004

Iron telluride ladder compounds: Predicting the structural and magnetic properties of BaFe 2 Te 3 journal, April 2020

Magnetic states of iron-based two-leg ladder tellurides journal, November 2019

Structure of the high-temperature form of osmium(IV) chloride journal, August 1977

Is the ground state of 5 d 4 double-perovskite Iridate Ba 2 YIrO 6 magnetic or nonmagnetic? journal, May 2018

Possible Anomalies at a Semimetal-Semiconductor Transistion journal, October 1968

Iridium double perovskite Sr 2 YIrO 6 : A combined structural and specific heat study journal, February 2017

Title: Magnetization dynamics fingerprints of an excitonic condensate $t_{2 g}^{4}$ magnet

Observation of spin-orbit excitations and Hund's multiplets in ${Ca}_{2} {RuO}_{4}$
journal, July 2019

On the possibility of excitonic magnetism in Ir double perovskites
journal, January 2016

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

Comparative Study of Potentially J _eff = 0 Ground State Iridium(V) in SrLaNiIrO ₆ , SrLaMgIrO ₆ , and SrLaZnIrO ₆: Comparative Study of Potentially J _eff = 0 Ground State Iridium(V) in SrLaNiIrO ₆ , SrLaMgIrO ₆ , and SrLaZnIrO ₆
journal, November 2017

Quantum magnetism of iron-based ladders: Blocks, spirals, and spin flux
journal, July 2021

Diluted paramagnetic impurities in nonmagnetic ${Ba}_{2} {YIrO}_{6}$
journal, October 2017

Interaction-induced topological phase transition and Majorana edge states in low-dimensional orbital-selective Mott insulators
journal, May 2021

Suppression of effective spin-orbit coupling by thermal fluctuations in spin-orbit coupled antiferromagnets
journal, July 2021

Novel Magnetism of ${Ir}^{5 +} (5 d^{4})$ Ions in the Double Perovskite ${Sr}_{2} {YIrO}_{6}$
journal, February 2014

Weakly coupled alternating $S = \frac{1}{2}$ chains in the distorted honeycomb lattice compound ${Na}_{2} {Cu}_{2} {TeO}_{6}$
journal, December 2020

Intertwined charge, spin, and pairing orders in doped iron ladders
journal, June 2021

Magnetic Excitation Spectra of ${Sr}_{2} {IrO}_{4}$ Probed by Resonant Inelastic X-Ray Scattering: Establishing Links to Cuprate Superconductors
journal, April 2012

Strong Coupling Nature of the Excitonic Insulator State in ${Ta}_{2} {NiSe}_{5}$
journal, June 2018

Excitonic condensation in systems of strongly correlated electrons
journal, July 2015

Density-matrix algorithms for quantum renormalization groups
journal, October 1993

Anisotropic uniaxial pressure response of the Mott insulator Ca $_{2}$ RuO $_{4}$
journal, November 2013

Excitonic quasiparticles in a spin–orbit Mott insulator
journal, July 2014

Structural and Magnetic Properties of the Iridium Double Perovskites Ba _{2– x} Sr _x YIrO ₆
journal, October 2015

Spectral functions with the density matrix renormalization group: Krylov-space approach for correction vectors
journal, November 2016

Magnetic states of the quasi-one-dimensional iron chalcogenide ${Ba}_{2} {FeS}_{3}$
journal, September 2021

The density matrix renormalization group for strongly correlated electron systems: A generic implementation
journal, September 2009

Orbital-selective Peierls phase in the metallic dimerized chain ${MoOCl}_{2}$
journal, August 2021

Fingerprints of an orbital-selective Mott phase in the block magnetic state of BaFe2Se3 ladders
journal, June 2019

First-principles study of the low-temperature charge density wave phase in the quasi-one-dimensional Weyl chiral compound $({TaSe}_{4})_{2} I$
journal, May 2020

Excitonic Magnetism in Van Vleck–type $d^{4}$ Mott Insulators
journal, November 2013

$J$ Freezing and Hund’s Rules in Spin-Orbit-Coupled Multiorbital Hubbard Models
journal, February 2017

Unraveling the Nature of Magnetism of the $5 d^{4}$ Double Perovskite ${Ba}_{2} {YIrO}_{6}$
journal, June 2018

Density matrix formulation for quantum renormalization groups
journal, November 1992

Spin-orbital entangled excitonic insulator with quadrupole order
journal, February 2019

Origin of magnetic moments and presence of spin-orbit singlets in ${Ba}_{2} {YIrO}_{6}$
journal, July 2018

Crystal and magnetic structure of ${Ca}_{2} {RuO}_{4} :$ Magnetoelastic coupling and the metal-insulator transition
journal, July 1998

Zero-gap semiconductor to excitonic insulator transition in Ta2NiSe5
journal, February 2017

Possible spin-orbit driven spin-liquid ground state in the double perovskite phase of Ba $_{3}$ YIr $_{2}$ O $_{9}$
journal, October 2013

Signatures of exciton condensation in a transition metal dichalcogenide
journal, December 2017

Origin of the Spin-Orbital Liquid State in a Nearly $J = 0$ Iridate ${Ba}_{3} {ZnIr}_{2} O_{9}$
journal, March 2016

Roles of Hund's rule coupling in excitonic density-wave states
journal, December 2014

Higgs mode and its decay in a two-dimensional antiferromagnet
journal, March 2017

Excitonic magnetism at the intersection of spin-orbit coupling and crystal-field splitting
journal, August 2020

Hopping-Induced Ground-State Magnetism in $6 H$ Perovskite Iridates
journal, July 2019

Strongly Enhanced Tunneling at Total Charge Neutrality in Double-Bilayer Graphene- ${WSe}_{2}$ Heterostructures
journal, April 2018

Excitonic Insulator
journal, June 1967

Magnetic phases for strongly correlated $t_{2 g}^{4}$ electrons on the square lattice: Impact of spin-orbit coupling and crystal field
journal, September 2021

The transition to the metallic state
journal, February 1961

Spin-Orbit Physics Giving Rise to Novel Phases in Correlated Systems: Iridates and Related Materials
journal, March 2016

Observation of heavy spin-orbit excitons propagating in a nonmagnetic background: The case of ${(Ba, Sr)}_{2} {YIrO}_{6}$
journal, February 2018

Dynamical correlation functions using the density matrix renormalization group
journal, July 1999

Effective magnetic interactions in spin-orbit coupled $d^{4}$ Mott insulators
journal, January 2017

Influence of structural distortions on the Ir magnetism in Ba2−xSrxYIrO6 double perovskites
journal, June 2016

Neutron and ARPES constraints on the couplings of the multiorbital Hubbard model for the iron pnictides
journal, September 2010

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

Magnetic phase transitions in quantum spin-orbital liquids
journal, April 2020

Magnetism out of antisite disorder in the $J = 0$ compound ${Ba}_{2} {YIrO}_{6}$
journal, October 2017

Highly Anisotropic Magnon Dispersion in ${Ca}_{2} {RuO}_{4}$ : Evidence for Strong Spin Orbit Coupling
journal, December 2015

Magnetic excitations in a spin-orbit-coupled $d^{4}$ Mott insulator on the square lattice
journal, July 2014

Novel Magnetic Block States in Low-Dimensional Iron-Based Superconductors
journal, July 2019

Density matrix renormalization group study of a three-orbital Hubbard model with spin-orbit coupling in one dimension
journal, October 2017

Study of electronic structure and magnetism in d4 double perovskite iridates A2ScIrO6 (A = Ba, Sr)
journal, December 2019

Theory of Superconductivity
journal, December 1957

Novel magnetic state in $d^{4}$ Mott insulators
journal, February 2015

Prediction of exotic magnetic states in the alkali-metal quasi-one-dimensional iron selenide compound ${Na}_{2} {FeSe}_{2}$
journal, July 2020

Spin-orbital excitons and their potential condensation in pentavalent iridates
journal, January 2019

Evidence for a low-temperature magnetic ground state in double-perovskite iridates with $I r^{5 +} (5 d^{4})$ ions
journal, August 2017

Giant exciton Fano resonance in quasi-one-dimensional ${Ta}_{2} {NiSe}_{5}$
journal, May 2017

Engineering 1D Quantum Stripes from Superlattices of 2D Layered Materials
journal, October 2016

${Ba}_{2} {YIrO}_{6}$ : A cubic double perovskite material with ${Ir}^{5 +}$ ions
journal, January 2016

Breakdown of $J = 0$ nonmagnetic state in $d^{4}$ iridate double perovskites: A first-principles study
journal, September 2015

Emergence of superconductivity in doped multiorbital Hubbard chains
journal, May 2020

The challenge of spin–orbit-tuned ground states in iridates: a key issues review
journal, February 2018

Mott transition, spin-orbit effects, and magnetism in ${Ca}_{2} {RuO}_{4}$
journal, February 2017

Spin–orbit effects in pentavalent iridates: models and materials
journal, August 2021

Bose–Einstein condensation of excitons in bilayer electron systems
journal, December 2004

Iron telluride ladder compounds: Predicting the structural and magnetic properties of ${BaFe}_{2} {Te}_{3}$
journal, April 2020

Magnetic states of iron-based two-leg ladder tellurides
journal, November 2019

Structure of the high-temperature form of osmium(IV) chloride
journal, August 1977

Is the ground state of 5 d 4 double-perovskite Iridate Ba 2 YIrO 6 magnetic or nonmagnetic?
journal, May 2018

Possible Anomalies at a Semimetal-Semiconductor Transistion
journal, October 1968

Iridium double perovskite ${Sr}_{2} {YIrO}_{6}$ : A combined structural and specific heat study
journal, February 2017

Spin-orbit coupling driven insulating state in hexagonal iridates $S r_{3} M Ir O_{6}$ ( $M = Sr, Na, Li$ )
journal, December 2018