Spin glass behavior in frustrated quantum spin system CuAl 2 O 4 with a possible orbital liquid state

Nirmala, R.; Jang, Kwang-Hyun; Sim, Hasung; Cho, Hwanbeom; Lee, Junghwan; Yang, Nam-Geun; Lee, Seongsu; Ibberson, R. M.; Kakurai, K.; Matsuda, M.; Cheong, S-W; Gapontsev, V. V.; Streltsov, S. V.; Park, Je-Geun

doi:10.1088/1361-648X/aa5c72

Title: Spin glass behavior in frustrated quantum spin system CuAl ₂ O ₄ with a possible orbital liquid state

Abstract

CuAl₂O₄ is a normal spinel oxide having quantum spin, S = 1/2 for Cu²⁺. It is a rather unique feature that the Cu²⁺ ions of CuAl₂O₄ sit at a tetrahedral position, not like the usual octahedral position for many oxides. At low temperatures, it exhibits all the thermodynamic evidence of a quantum spin glass. For example, the polycrystalline CuAl₂O₄ shows a cusp centered at ~2 K in the low-field dc magnetization data and a clear frequency dependence in the ac magnetic susceptibility while it displays logarithmic relaxation behavior in a time dependence of the magnetization. At the same time, there is a peak at ~2.3 K in the heat capacity, which shifts towards a higher temperature with magnetic fields. Conversely, there is no evidence of new superlattice peaks in the high-resolution neutron powder diffraction data when cooled from 40 to 0.4 K. This implies that there is no long-ranged magnetic order down to 0.4 K, thus confirming a spin glass-like ground state for CuAl₂O₄. Interestingly, there is no sign of structural distortion either although Cu²⁺ is a Jahn–Teller active ion. Therefore, we claim that an orbital liquid state is the most likely ground state in CuAl₂O₄. Of further interest, itmore »« less

Authors:

Nirmala, R. ^[1]; Jang, Kwang-Hyun ^[2]; Sim, Hasung ^[3]; Cho, Hwanbeom ^[3]; Lee, Junghwan ^[2]; Yang, Nam-Geun ^[2]; Lee, Seongsu ^[4]; Ibberson, R. M. ^[5]; Kakurai, K. ^[6]; Matsuda, M. ^[7]; Cheong, S-W ^[8]; Gapontsev, V. V. ^[9]; Streltsov, S. V. ^[10]; Park, Je-Geun ^[11]

Seoul National Univ. (Korea, Republic of). Center for Stronly Correlated Materials Research; Indian Inst. of Technology (IIT), Madras (India). Dept. of Physics; Sungkyunkwan Univ., Suwon (Republic of Korea). Dept. of Physics
Seoul National Univ. (Korea, Republic of). Center for Stronly Correlated Materials Research; Sungkyunkwan Univ., Suwon (Republic of Korea). Dept. of Physics
Inst. for Basic Science, Seoul (Korea, Republic of). Center for Correlated Electron Systems; Seoul National Univ. (Korea, Republic of). Dept. of Physics and Astronomy
Korea Atomic Energy Research Inst., Daejeon (Korea, Republic of). Neturon Science Division; Rutgers Univ., Piscataway, NJ (United States). Rutgers Center for Emergent Materials and Dept. of Physics and Astronomy
ISIS Facility, Didcot (United Kingdom). Rutherford Appleton Lab.; Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical and Engineering Materials
Japan Atomic Energy Agency (JAEA), Tokai (Japan). Quantum Beam Science Center
Japan Atomic Energy Agency (JAEA), Tokai (Japan). Quantum Beam Science Center; Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Quantum Condensed Matter Division
Rutgers Univ., Piscataway, NJ (United States). Rutgers Center for Emergent Materials and Dept. of Physics and Astronomy
Russian Academy of Sciences (RAS), Ekaterinburg (Russian Federation). MN Miheev Inst. of Metal Physics of Ural Branch
Russian Academy of Sciences (RAS), Ekaterinburg (Russian Federation). MN Miheev Inst. of Metal Physics of Ural Branch; Ural Federal Univ., Ekaterinburg (Russia)
Seoul National Univ. (Korea, Republic of). Center for Stronly Correlated Materials Research; Sungkyunkwan Univ., Suwon (Republic of Korea). Dept. of Physics; Inst. for Basic Science, Seoul (Korea, Republic of). Center for Correlated Electron Systems; Seoul National Univ. (Korea, Republic of). Dept. of Physics and Astronomy

Publication Date:: 2017-02-15

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

Sponsoring Org.:: USDOE

OSTI Identifier:: 1346686

Grant/Contract Number:: AC05-00OR22725; FG02-07ER46382

Resource Type:: Accepted Manuscript

Journal Name:: Journal of Physics. Condensed Matter

Additional Journal Information:: Journal Volume: 29; Journal Issue: 13; Journal ID: ISSN 0953-8984

Publisher:: IOP Publishing

Country of Publication:: United States

Language:: English

Subject:: 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; quantum spin system; frustration; spin glass; orbital liquid state

Citation Formats


                    Nirmala, R., Jang, Kwang-Hyun, Sim, Hasung, Cho, Hwanbeom, Lee, Junghwan, Yang, Nam-Geun, Lee, Seongsu, Ibberson, R. M., Kakurai, K., Matsuda, M., Cheong, S-W, Gapontsev, V. V., Streltsov, S. V., and Park, Je-Geun. Spin glass behavior in frustrated quantum spin system CuAl 2 O 4 with a possible orbital liquid state.  United States: N. p., 2017. 
Web.  doi:10.1088/1361-648X/aa5c72.

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                    Nirmala, R., Jang, Kwang-Hyun, Sim, Hasung, Cho, Hwanbeom, Lee, Junghwan, Yang, Nam-Geun, Lee, Seongsu, Ibberson, R. M., Kakurai, K., Matsuda, M., Cheong, S-W, Gapontsev, V. V., Streltsov, S. V., & Park, Je-Geun. Spin glass behavior in frustrated quantum spin system CuAl 2 O 4 with a possible orbital liquid state.  United States.  https://doi.org/10.1088/1361-648X/aa5c72

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                    Nirmala, R., Jang, Kwang-Hyun, Sim, Hasung, Cho, Hwanbeom, Lee, Junghwan, Yang, Nam-Geun, Lee, Seongsu, Ibberson, R. M., Kakurai, K., Matsuda, M., Cheong, S-W, Gapontsev, V. V., Streltsov, S. V., and Park, Je-Geun. Wed .  
"Spin glass behavior in frustrated quantum spin system CuAl 2 O 4 with a possible orbital liquid state".  United States.  https://doi.org/10.1088/1361-648X/aa5c72.  https://www.osti.gov/servlets/purl/1346686.

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@article{osti_1346686,

  title        = {Spin glass behavior in frustrated quantum spin system CuAl 2 O 4 with a possible orbital liquid state},

  author       = {Nirmala, R. and Jang, Kwang-Hyun and Sim, Hasung and Cho, Hwanbeom and Lee, Junghwan and Yang, Nam-Geun and Lee, Seongsu and Ibberson, R. M. and Kakurai, K. and Matsuda, M. and Cheong, S-W and Gapontsev, V. V. and Streltsov, S. V. and Park, Je-Geun},

  abstractNote = {CuAl2O4 is a normal spinel oxide having quantum spin, S = 1/2 for Cu2+. It is a rather unique feature that the Cu2+ ions of CuAl2O4 sit at a tetrahedral position, not like the usual octahedral position for many oxides. At low temperatures, it exhibits all the thermodynamic evidence of a quantum spin glass. For example, the polycrystalline CuAl2O4 shows a cusp centered at ~2 K in the low-field dc magnetization data and a clear frequency dependence in the ac magnetic susceptibility while it displays logarithmic relaxation behavior in a time dependence of the magnetization. At the same time, there is a peak at ~2.3 K in the heat capacity, which shifts towards a higher temperature with magnetic fields. Conversely, there is no evidence of new superlattice peaks in the high-resolution neutron powder diffraction data when cooled from 40 to 0.4 K. This implies that there is no long-ranged magnetic order down to 0.4 K, thus confirming a spin glass-like ground state for CuAl2O4. Interestingly, there is no sign of structural distortion either although Cu2+ is a Jahn–Teller active ion. Therefore, we claim that an orbital liquid state is the most likely ground state in CuAl2O4. Of further interest, it also exhibits a large frustration parameter, f = |θ CW/T m| ~ 67, one of the largest values reported for spinel oxides. These observations suggest that CuAl2O4 should be a rare example of a frustrated quantum spin glass with a good candidate for an orbital liquid state.},

  doi          = {10.1088/1361-648X/aa5c72},

  journal      = {Journal of Physics. Condensed Matter},

  number       = 13,

  volume       = 29,

  place        = {United States},

  year         = {2017},

  month        = {2}

}

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Works referencing / citing this record:

Field-cooling induced giant vertical magnetization shift in frustrated low dimensional spin-chain Sr ₃ NiIrO ₆ system
journal, August 2019

Krishnamurthy, J.; Anil Kumar, P. S.
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Theoretical evidence of spin-orbital-entangled $J_{eff} = \frac{1}{2}$ state in the $3 d$ transition metal oxide ${CuAl}_{2} O_{4}$
journal, October 2019

Kim, Choong H.; Baidya, Santu; Cho, Hwanbeom
Physical Review B, Vol. 100, Issue 16
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Title: Spin glass behavior in frustrated quantum spin system CuAl 2 O 4 with a possible orbital liquid state

Abstract

Citation Formats

Ferromagnet or spin glass? Magnetic ordering in Au-Fe alloys journal, May 1974

Cation distribution and bond lengths in CoAl2O4 spinel journal, October 2003

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

Zero-point entropy in ‘spin ice’ journal, May 1999

Emergent excitations in a geometrically frustrated magnet journal, August 2002

Ordering and Antiferromagnetism in Ferrites journal, May 1956

Pressure-dependent magnetic properties of geometrically frustrated ZnCr 2 O 4 journal, November 2005

Magnetic properties of normal spinels with only a-a interactions journal, January 1964

Spin and Orbital Frustration in MnSc 2 S 4 and FeSc 2 S 4 journal, March 2004

Order-by-disorder and spiral spin-liquid in frustrated diamond-lattice antiferromagnets journal, May 2007

Kinetically inhibited order in a diamond-lattice antiferromagnet journal, September 2011

Geometric frustration in the cubic spinels M Al 2 O 4 ( M = Co , Fe, and Mn) journal, November 2005

Melting of antiferromagnetic ordering in spinel oxide CoAl 2 O 4 journal, March 2007

Approaching the true ground state of frustrated A -site spinels: A combined magnetization and polarized neutron scattering study journal, May 2014

Spin liquid in a single crystal of the frustrated diamond lattice antiferromagnet CoAl 2 O 4 journal, September 2011

Spin-glass state in CuGa 2 O 4 journal, April 2001

Zero-point entropy of the spinel spin glasses CuGa 2 O 4 and CuAl 2 O 4 journal, January 2009

Nanostructured CuAl2O4: Co-precipitation synthesis, optical and photocatalytic properties journal, September 2016

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

Structural study of copper-nickel aluminate (CuxNi1−xAl2O4) spinels journal, November 1985

Synthesis and magnetic properties of nano-dimensional Fe 1−x Cu x Al 2 O 4 (0.3 ≤ x ≤ 0.8) journal, January 2015

Strong frustration and dilution-enhanced order in a quasi-2D spin glass journal, April 1990

Orbital physics in sulfur spinels: ordered, liquid and glassy ground states journal, January 2004

Spin-glass state of ( N d , L a ) 0.5 Sr 1.5 MnO 4 journal, December 2000

Spin glasses: Experimental facts, theoretical concepts, and open questions journal, October 1986

Electrical and magnetic properties of R2Mo2O7 (R=Nd, Sm, Gd and Dy) journal, April 2003

Structure Solution of the High-Pressure Phase of CuWO 4 and Evolution of the Jahn–Teller Distortion journal, September 2011

Explicit, First-Principles Tight-Binding Theory journal, December 1984

Crystal-field splitting for low symmetry systems in ab initio calculations journal, June 2005

Density-functional theory and strong interactions: Orbital ordering in Mott-Hubbard insulators journal, August 1995

Spin-Orbital Short-Range Order on a Honeycomb-Based Lattice journal, May 2012

Absence of Jahn−Teller transition in the hexagonal Ba 3 CuSb 2 O 9 single crystal journal, July 2015

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Title: Spin glass behavior in frustrated quantum spin system CuAl ₂ O ₄ with a possible orbital liquid state

Ferromagnet or spin glass? Magnetic ordering in Au-Fe alloys
journal, May 1974

Cation distribution and bond lengths in CoAl2O4 spinel
journal, October 2003

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

Zero-point entropy in ‘spin ice’
journal, May 1999

Emergent excitations in a geometrically frustrated magnet
journal, August 2002

Ordering and Antiferromagnetism in Ferrites
journal, May 1956

Pressure-dependent magnetic properties of geometrically frustrated ${ZnCr}_{2} O_{4}$
journal, November 2005

Magnetic properties of normal spinels with only a-a interactions
journal, January 1964

Spin and Orbital Frustration in ${MnSc}_{2} S_{4}$ and ${FeSc}_{2} S_{4}$
journal, March 2004

Order-by-disorder and spiral spin-liquid in frustrated diamond-lattice antiferromagnets
journal, May 2007

Kinetically inhibited order in a diamond-lattice antiferromagnet
journal, September 2011

Geometric frustration in the cubic spinels $M {Al}_{2} O_{4}$ ( $M = Co$ , Fe, and Mn)
journal, November 2005

Melting of antiferromagnetic ordering in spinel oxide CoAl ₂ O ₄
journal, March 2007

Approaching the true ground state of frustrated $A$ -site spinels: A combined magnetization and polarized neutron scattering study
journal, May 2014

Spin liquid in a single crystal of the frustrated diamond lattice antiferromagnet CoAl $_{2}$ O $_{4}$
journal, September 2011

Spin-glass state in ${CuGa}_{2} O_{4}$
journal, April 2001

Zero-point entropy of the spinel spin glasses CuGa ₂ O ₄ and CuAl ₂ O ₄
journal, January 2009

Nanostructured CuAl2O4: Co-precipitation synthesis, optical and photocatalytic properties
journal, September 2016

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

Structural study of copper-nickel aluminate (CuxNi1−xAl2O4) spinels
journal, November 1985

Synthesis and magnetic properties of nano-dimensional Fe _1−x Cu _x Al ₂ O ₄ (0.3 ≤ x ≤ 0.8)
journal, January 2015

Strong frustration and dilution-enhanced order in a quasi-2D spin glass
journal, April 1990

Orbital physics in sulfur spinels: ordered, liquid and glassy ground states
journal, January 2004

Spin-glass state of ${(N d, L a)}_{0.5} {Sr}_{1.5} {MnO}_{4}$
journal, December 2000

Spin glasses: Experimental facts, theoretical concepts, and open questions
journal, October 1986

Electrical and magnetic properties of R2Mo2O7 (R=Nd, Sm, Gd and Dy)
journal, April 2003

Structure Solution of the High-Pressure Phase of CuWO ₄ and Evolution of the Jahn–Teller Distortion
journal, September 2011

Explicit, First-Principles Tight-Binding Theory
journal, December 1984

Crystal-field splitting for low symmetry systems in ab initio calculations
journal, June 2005

Density-functional theory and strong interactions: Orbital ordering in Mott-Hubbard insulators
journal, August 1995

Spin-Orbital Short-Range Order on a Honeycomb-Based Lattice
journal, May 2012

Absence of Jahn−Teller transition in the hexagonal Ba ₃ CuSb ₂ O ₉ single crystal
journal, July 2015

Ground state and low-energy magnetic dynamics in the frustrated magnet ${CoAl}_{2} O_{4}$ as revealed by local spin probes
journal, April 2015

Field-cooling induced giant vertical magnetization shift in frustrated low dimensional spin-chain Sr ₃ NiIrO ₆ system
journal, August 2019

Theoretical evidence of spin-orbital-entangled $J_{eff} = \frac{1}{2}$ state in the $3 d$ transition metal oxide ${CuAl}_{2} O_{4}$
journal, October 2019