Realization of the orbital-selective Mott state at the molecular level in Ba 3 LaRu 2 O 9

Chen, Q.; Verrier, A.; Ziat, D.; Clune, A. J.; Rouane, R.; Bazier-Matte, X.; Wang, G.; Calder, Stuart; Taddei, Keith M.; Cruz, Clarina R. dela; Kolesnikov, Alexander I.; Ma, J.; Cheng, J. -G.; Liu, Z.; Quilliam, J. A.; Musfeldt, J. L.; Zhou, H. D.; Aczel, Adam A.

doi:10.1103/PhysRevMaterials.4.064409

Title: Realization of the orbital-selective Mott state at the molecular level in ${Ba}_{3} {LaRu}_{2} O_{9}$

Abstract

Molecular magnets based on heavy transition metals have recently attracted significant interest in the quest for novel magnetic properties. For systems with an odd number of valence electrons per molecule, high or low molecular spin states are typically expected in the double exchange or quasi-molecular orbital limits respectively. In this work, we use bulk characterization, muon spin relaxation, neutron diffraction, and inelastic neutron scattering to identify a rare intermediate spin-3/2 per dimer state in the 6H-perovskite Ba3LaRu2O9 that cannot be understood in a double exchange or quasi-molecular orbital picture and instead arises from orbital-selective Mott insulating behavior at the molecular level. Our measurements are also indicative of collinear stripe magnetic order below TN = 26(1) K for these molecular spin-3/2 degrees-of-freedom, which is consistent with expectations for an ideal triangular lattice with significant next nearest neighbor in-plane exchange. Finally, we present neutron diffraction and Raman scattering data under applied pressure that reveal low-lying structural and spin state transitions at modest pressures P < 1 GPa, which highlights the delicate balance between competing energy scales in this system.

Authors:

^[1];

^[2]; Ziat, D. ^[2];

^[1]; Rouane, R. ^[2]; Bazier-Matte, X. ^[2]; Wang, G. ^[3];

^[4]; Taddei, Keith M. ^[4];

^[4];

^[3];

^[5]; Liu, Z. ^[6];

^[2]; Musfeldt, J. L. ^[1]; Zhou, H. D. ^[1];

^[7]

Univ. of Tennessee, Knoxville, TN (United States)
Univ. de Sherbrooke, Sherbrooke, Quebec (Canada). Inst. Quantique and Departement de Physique
Shanghai Jiao Tong Univ. (China). Key Lab. of Artificial Structures and Quantum Control
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Chinese Academy of Sciences, Beijing (China). Beijing National Lab. for Condensed Matter Physics and Inst. of Physics; Songshan Lake Materials Lab., Dongguan, Guangdong (China)
Univ. of Illinois, Chicago, IL (United States)
Univ. of Tennessee, Knoxville, TN (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

Publication Date:: Tue Jun 09 00:00:00 EDT 2020

Research Org.:: Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Illinois at Chicago, IL (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

OSTI Identifier:: 1694394

Alternate Identifier(s):: OSTI ID: 1778253

Grant/Contract Number:: AC05-00OR22725; NA0003975

Resource Type:: Accepted Manuscript

Journal Name:: Physical Review Materials

Additional Journal Information:: Journal Volume: 4; Journal Issue: 6; Journal ID: ISSN 2475-9953

Publisher:: American Physical Society (APS)

Country of Publication:: United States

Language:: English

Subject:: 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; Magnetic order; Magnetic phase transitions; Molecular magnetism

Citation Formats


                    Chen, Q., Verrier, A., Ziat, D., Clune, A. J., Rouane, R., Bazier-Matte, X., Wang, G., Calder, Stuart, Taddei, Keith M., Cruz, Clarina R. dela, Kolesnikov, Alexander I., Ma, J., Cheng, J. -G., Liu, Z., Quilliam, J. A., Musfeldt, J. L., Zhou, H. D., and Aczel, Adam A. Realization of the orbital-selective Mott state at the molecular level in Ba 3 LaRu 2 O 9.  United States: N. p., 2020. 
Web.  doi:10.1103/PhysRevMaterials.4.064409.

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                    Chen, Q., Verrier, A., Ziat, D., Clune, A. J., Rouane, R., Bazier-Matte, X., Wang, G., Calder, Stuart, Taddei, Keith M., Cruz, Clarina R. dela, Kolesnikov, Alexander I., Ma, J., Cheng, J. -G., Liu, Z., Quilliam, J. A., Musfeldt, J. L., Zhou, H. D., & Aczel, Adam A. Realization of the orbital-selective Mott state at the molecular level in Ba 3 LaRu 2 O 9.  United States.  https://doi.org/10.1103/PhysRevMaterials.4.064409

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                    Chen, Q., Verrier, A., Ziat, D., Clune, A. J., Rouane, R., Bazier-Matte, X., Wang, G., Calder, Stuart, Taddei, Keith M., Cruz, Clarina R. dela, Kolesnikov, Alexander I., Ma, J., Cheng, J. -G., Liu, Z., Quilliam, J. A., Musfeldt, J. L., Zhou, H. D., and Aczel, Adam A. Tue .  
"Realization of the orbital-selective Mott state at the molecular level in Ba 3 LaRu 2 O 9".  United States.  https://doi.org/10.1103/PhysRevMaterials.4.064409.  https://www.osti.gov/servlets/purl/1694394.

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@article{osti_1694394,

  title        = {Realization of the orbital-selective Mott state at the molecular level in Ba 3 LaRu 2 O 9},

  author       = {Chen, Q. and Verrier, A. and Ziat, D. and Clune, A. J. and Rouane, R. and Bazier-Matte, X. and Wang, G. and Calder, Stuart and Taddei, Keith M. and Cruz, Clarina R. dela and Kolesnikov, Alexander I. and Ma, J. and Cheng, J. -G. and Liu, Z. and Quilliam, J. A. and Musfeldt, J. L. and Zhou, H. D. and Aczel, Adam A.},

  abstractNote = {Molecular magnets based on heavy transition metals have recently attracted significant interest in the quest for novel magnetic properties. For systems with an odd number of valence electrons per molecule, high or low molecular spin states are typically expected in the double exchange or quasi-molecular orbital limits respectively. In this work, we use bulk characterization, muon spin relaxation, neutron diffraction, and inelastic neutron scattering to identify a rare intermediate spin-3/2 per dimer state in the 6H-perovskite Ba3LaRu2O9 that cannot be understood in a double exchange or quasi-molecular orbital picture and instead arises from orbital-selective Mott insulating behavior at the molecular level. Our measurements are also indicative of collinear stripe magnetic order below TN = 26(1) K for these molecular spin-3/2 degrees-of-freedom, which is consistent with expectations for an ideal triangular lattice with significant next nearest neighbor in-plane exchange. Finally, we present neutron diffraction and Raman scattering data under applied pressure that reveal low-lying structural and spin state transitions at modest pressures P < 1 GPa, which highlights the delicate balance between competing energy scales in this system.},

  doi          = {10.1103/PhysRevMaterials.4.064409},

  journal      = {Physical Review Materials},

  number       = 6,

  volume       = 4,

  place        = {United States},

  year         = {Tue Jun 09 00:00:00 EDT 2020},

  month        = {Tue Jun 09 00:00:00 EDT 2020}

}

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Title: Realization of the orbital-selective Mott state at the molecular level in Ba 3 LaRu 2 O 9

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Orbital physics in transition metal compounds: new trends journal, November 2017

Specific heat data of high-Tc superconductors: Lattice and electronic contributions journal, February 1989

Observation of an Unconventional Metal-Insulator Transition in Overdoped C u O 2 Compounds journal, August 2002

Spin gap and the nature of the 4 d 3 magnetic ground state in the frustrated fcc antiferromagnet Ba 2 YRuO 6 journal, July 2013

Exotic Magnetic Order in the Orbital-Selective Mott Regime of Multiorbital Systems journal, March 2014

Orbital-Selective Mott Transitions in the Degenerate Hubbard Model journal, May 2004

Orbital-selective insulator-metal transition in V 2 O 3 under external pressure journal, January 2006

Subband Filling and Mott Transition in Ca 2 − x Sr x RuO 4 journal, May 2007

U ( 1 ) slave-spin theory and its application to Mott transition in a multiorbital model for iron pnictides journal, August 2012

A suite-level review of the neutron powder diffraction instruments at Oak Ridge National Laboratory journal, September 2018

Charge Order at the Frontier between the Molecular and Solid States in Ba 3 NaRu 2 O 9 journal, May 2012

Specific heat of single-crystal PrMnO 3 journal, September 2005

A new protocol for the determination of magnetic structures using simulated annealing and representational analysis (SARAh) journal, March 2000

Spin-orbital interaction for face-sharing octahedra: Realization of a highly symmetric SU(4) model journal, April 2015

Orbital-Selective Mott Transition out of Band Degeneracy Lifting journal, March 2009

Crystal Structures and Magnetic Properties of 6H-Perovskites Ba3MRu2O9 (M=Y, In, La, Sm, Eu, and Lu) journal, May 2002

Fermi Surface Topology of C a 1.5 S r 0.5 R u O 4 Determined by Angle-Resolved Photoelectron Spectroscopy journal, October 2004

Observation of the Pressure Dependent Reversible Enhancement ofTc and Loss of the Anomalous Constricted Hysteresis for [Ru2(O2CMe)4]3[Cr(CN)6] journal, October 2007

Frustrated spin- 1 2 molecular magnetism in the mixed-valence antiferromagnets Ba 3 M Ru 2 O 9 ( M = In , Y, Lu) journal, May 2017

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

Non-Fermi-Liquid Behavior and Double-Exchange Physics in Orbital-Selective Mott Systems journal, November 2005

Muon-spin-rotation experiments in orthoferrites journal, May 1983

Orbital-selective Mott-insulator transition in Ca 2 - x Sr x RuO 4 journal, February 2002

Title: Realization of the orbital-selective Mott state at the molecular level in ${Ba}_{3} {LaRu}_{2} O_{9}$

Magnetic properties of quadruple perovskites Ba4LnRu3O12 (Ln=La, Nd, Sm–Gd, Dy–Lu)
journal, January 2010

Magnetically driven orbital-selective insulator–metal transition in double perovskite oxides
journal, November 2018

Observation of a Novel Orbital Selective Mott Transition in ${Ca}_{1.8} {Sr}_{0.2} {RuO}_{4}$
journal, August 2009

SEQUOIA: A Newly Operating Chopper Spectrometer at the SNS
journal, November 2010

Pressure-driven high-to-low spin transition in the bimetallic quantum magnet $[{Ru}_{2} (O_{2} CMe)_{4}]_{3} [Cr (CN)_{6}]$
journal, September 2014

Magnetoelastic coupling in [Ru $_{2}$ (O $_{2}$ CMe) $_{4}$ ] $_{3}$ [Cr(CN) $_{6}$ ] molecule-based magnet
journal, December 2012

Exotic Magnetism on the Quasi-fcc Lattices of the $d^{3}$ Double Perovskites ${La}_{2} Na B^{'} O_{6}$ ( $B^{'} = Ru$ , Os)
journal, March 2014

Block Magnetic Excitations in the Orbitally Selective Mott Insulator ${BaFe}_{2} {Se}_{3}$
journal, July 2015

Recent advances in magnetic structure determination by neutron powder diffraction
journal, October 1993

Competition between supersolid phases and magnetization plateaus in the frustrated easy-axis antiferromagnet on a triangular lattice
journal, April 2011

Orbital-Selective Mott Phase in Multiorbital Models for Alkaline Iron Selenides $K_{1 - x} {Fe}_{2 - y} {Se}_{2}$
journal, April 2013

Quantum phase transition between orbital-selective Mott states in Hund's metals
journal, December 2014

Orbital-dependent singlet dimers and orbital-selective Peierls transitions in transition-metal compounds
journal, April 2014

Tunable Quantum Spin Liquidity in the $1 / 6$ th-Filled Breathing Kagome Lattice
journal, May 2018

Spin-orbit coupling controlled ground state in ${Sr}_{2} {ScOsO}_{6}$
journal, June 2016

Novel Mott Transitions in a Nonisotropic Two-Band Hubbard Model
journal, September 2005

Possible valence-bond condensation in the frustrated cluster magnet LiZn2Mo3O8
journal, May 2012

Spin dynamics of the block orbital-selective Mott phase
journal, September 2018

High-spin ground states via electron delocalization in mixed-valence imidazolate-bridged divanadium complexes
journal, March 2010

Severe Fermi Surface Reconstruction at a Metamagnetic Transition in ${Ca}_{2 - x} {Sr}_{x} {RuO}_{4}$ (for $0.2 \leq x \leq 0.5$ )
journal, November 2005

Dynamical behavior across the Mott transition of two bands with different bandwidths
journal, November 2005

Large Positive Zero-Field Splitting in the Cluster Magnet Ba ₃ CeRu ₂ O ₉
journal, May 2019

Spin orders and lattice distortions of geometrically frustrated 6H-perovskites Ba $_{3} B^{'}$ Ru $_{2}$ O $_{9}$ ( $B^{'}$ = La $^{3 +}$ , Nd $^{3 +}$ , and Y $^{3 +}$ )
journal, April 2013

Orbital-selective Mott transition in multiband systems: Slave-spin representation and dynamical mean-field theory
journal, November 2005

Molecular Quantum Magnetism in ${LiZn}_{2} {Mo}_{3} O_{8}$
journal, January 2014

Orbital physics in transition metal compounds: new trends
journal, November 2017

Specific heat data of high-Tc superconductors: Lattice and electronic contributions
journal, February 1989

Observation of an Unconventional Metal-Insulator Transition in Overdoped ${C u O}_{2}$ Compounds
journal, August 2002

Spin gap and the nature of the 4 $d^{3}$ magnetic ground state in the frustrated fcc antiferromagnet Ba $_{2}$ YRuO $_{6}$
journal, July 2013

Exotic Magnetic Order in the Orbital-Selective Mott Regime of Multiorbital Systems
journal, March 2014

Orbital-Selective Mott Transitions in the Degenerate Hubbard Model
journal, May 2004

Orbital-selective insulator-metal transition in $V_{2} O_{3}$ under external pressure
journal, January 2006

Subband Filling and Mott Transition in ${Ca}_{2 - x} {Sr}_{x} {RuO}_{4}$
journal, May 2007

$U (1)$ slave-spin theory and its application to Mott transition in a multiorbital model for iron pnictides
journal, August 2012

A suite-level review of the neutron powder diffraction instruments at Oak Ridge National Laboratory
journal, September 2018

Charge Order at the Frontier between the Molecular and Solid States in ${Ba}_{3} {NaRu}_{2} O_{9}$
journal, May 2012

Specific heat of single-crystal PrMnO ₃
journal, September 2005

A new protocol for the determination of magnetic structures using simulated annealing and representational analysis (SARAh)
journal, March 2000

Spin-orbital interaction for face-sharing octahedra: Realization of a highly symmetric SU(4) model
journal, April 2015

Orbital-Selective Mott Transition out of Band Degeneracy Lifting
journal, March 2009

Crystal Structures and Magnetic Properties of 6H-Perovskites Ba3MRu2O9 (M=Y, In, La, Sm, Eu, and Lu)
journal, May 2002

Fermi Surface Topology of ${C a}_{1.5} {S r}_{0.5} {R u O}_{4}$ Determined by Angle-Resolved Photoelectron Spectroscopy
journal, October 2004

Observation of the Pressure Dependent Reversible Enhancement ofTc and Loss of the Anomalous Constricted Hysteresis for [Ru2(O2CMe)4]3[Cr(CN)6]
journal, October 2007

Frustrated spin- $\frac{1}{2}$ molecular magnetism in the mixed-valence antiferromagnets ${Ba}_{3} M {Ru}_{2} O_{9} (M = In$ , Y, Lu)
journal, May 2017

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

Non-Fermi-Liquid Behavior and Double-Exchange Physics in Orbital-Selective Mott Systems
journal, November 2005

Muon-spin-rotation experiments in orthoferrites
journal, May 1983

Orbital-selective Mott-insulator transition in Ca 2 - x Sr x RuO 4
journal, February 2002