Magnetic and structural properties of the solid solution CuAl2(1–x)Ga2xO4

Bullard, Thomas J.; Susner, Michael A.; Taddei, Keith M.; Brant, J. A.; Haugan, T. J.

doi:10.1038/s41598-021-89197-1

Title: Magnetic and structural properties of the solid solution CuAl_2(1–x)Ga_2xO₄

Abstract

CuAl₂O₄ is a ternary oxide spinel with Cu²⁺ ions (s = 1/2) primarily populating the A-site diamond sublattice. The compound is reported to display evidence of spin glass behavior but possess a non-frozen magnetic ground state below the transition temperature. On the other hand, the spinel CuGa₂O₄ displays spin glass behavior at ~ 2.5 K with Cu²⁺ ions more readily tending to the B-site pyrochlore sublattice. Therefore, we investigate the magnetic and structural properties of the solid solution CuAl_2(1-x)Ga_2xO₄ examining the evolution of the magnetic behavior as Al³⁺ is replaced with a much larger Ga³⁺ ion. Our results show that the Cu²⁺ ions tend to migrate from tetrahedral to octahedral sites as the Ga³⁺ ion concentration increases, resulting in a concomitant change in the glassy magnetic properties of the solution. Results indicate glassy behavior for much of the solution with a general trend towards decreasing magnetic frustration as the Cu²⁺ ion shifts to the B-site. However, the x = 0.1 and 0.2 members of the system do not show glassy behavior down to our measurement limit (1.9 K) suggesting a delayed spin glass transition. We suggest that these two members are additional candidates for investigation to access highly frustrated exoticmore » quantum states.« less

Authors:

Bullard, Thomas J. ^[1];

^[1];

^[2]; Brant, J. A. ^[3]; Haugan, T. J. ^[3]

UES, Inc., Dayton, OH (United States); Wright-Patterson AFB, Dayton, OH (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Wright-Patterson AFB, Dayton, OH (United States)

Publication Date:: Mon May 31 00:00:00 EDT 2021

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

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

OSTI Identifier:: 1817392

Grant/Contract Number:: AC05-00OR22725; AC02-06CH11357

Resource Type:: Accepted Manuscript

Journal Name:: Scientific Reports

Additional Journal Information:: Journal Volume: 11; Journal Issue: 1; Journal ID: ISSN 2045-2322

Publisher:: Nature Publishing Group

Country of Publication:: United States

Language:: English

Subject:: 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; Condensed-matter physics; Magnetic properties and materials; Physics

Citation Formats


                    Bullard, Thomas J., Susner, Michael A., Taddei, Keith M., Brant, J. A., and Haugan, T. J. Magnetic and structural properties of the solid solution CuAl2(1–x)Ga2xO4.  United States: N. p., 2021. 
Web.  doi:10.1038/s41598-021-89197-1.

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                    Bullard, Thomas J., Susner, Michael A., Taddei, Keith M., Brant, J. A., & Haugan, T. J. Magnetic and structural properties of the solid solution CuAl2(1–x)Ga2xO4.  United States.  https://doi.org/10.1038/s41598-021-89197-1

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                    Bullard, Thomas J., Susner, Michael A., Taddei, Keith M., Brant, J. A., and Haugan, T. J. Mon .  
"Magnetic and structural properties of the solid solution CuAl2(1–x)Ga2xO4".  United States.  https://doi.org/10.1038/s41598-021-89197-1.  https://www.osti.gov/servlets/purl/1817392.

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@article{osti_1817392,

  title        = {Magnetic and structural properties of the solid solution CuAl2(1–x)Ga2xO4},

  author       = {Bullard, Thomas J. and Susner, Michael A. and Taddei, Keith M. and Brant, J. A. and Haugan, T. J.},

  abstractNote = {CuAl2O4 is a ternary oxide spinel with Cu2+ ions (s = 1/2) primarily populating the A-site diamond sublattice. The compound is reported to display evidence of spin glass behavior but possess a non-frozen magnetic ground state below the transition temperature. On the other hand, the spinel CuGa2O4 displays spin glass behavior at ~ 2.5 K with Cu2+ ions more readily tending to the B-site pyrochlore sublattice. Therefore, we investigate the magnetic and structural properties of the solid solution CuAl2(1-x)Ga2xO4 examining the evolution of the magnetic behavior as Al3+ is replaced with a much larger Ga3+ ion. Our results show that the Cu2+ ions tend to migrate from tetrahedral to octahedral sites as the Ga3+ ion concentration increases, resulting in a concomitant change in the glassy magnetic properties of the solution. Results indicate glassy behavior for much of the solution with a general trend towards decreasing magnetic frustration as the Cu2+ ion shifts to the B-site. However, the x = 0.1 and 0.2 members of the system do not show glassy behavior down to our measurement limit (1.9 K) suggesting a delayed spin glass transition. We suggest that these two members are additional candidates for investigation to access highly frustrated exotic quantum states.},

  doi          = {10.1038/s41598-021-89197-1},

  journal      = {Scientific Reports},

  number       = 1,

  volume       = 11,

  place        = {United States},

  year         = {Mon May 31 00:00:00 EDT 2021},

  month        = {Mon May 31 00:00:00 EDT 2021}

}

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Title: Magnetic and structural properties of the solid solution CuAl2(1–x)Ga2xO4

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Spin Glass Order by Antisite Disorder in the Highly Frustrated Spinel Oxide CoAl ₂ O ₄
journal, February 2013

Temperature dependence of the cation distribution in CuAl2O4 spinel [Temperature dependence of the cation distribution in CuAl2O4 spinel]
journal, July 2005

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

Low-temperature dynamic magnetic properties of PdxCo50Al50−x alloys
journal, February 1997

Dynamics of an Ising Spin-Glass in the Vicinity of the Spin-Glass Temperature
journal, August 1988

Evolution of magnetic and orbital properties in the magnetically diluted $A$ -site spinel ${Cu}_{1 - x} {Zn}_{x} {Rh}_{2} O_{4}$
journal, June 2018

Stability of the Sherrington-Kirkpatrick solution of a spin glass model
journal, May 1978

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

Dynamic critical behaviour of the CdCr2×0.85In2×0.15S4 spin-glass
journal, April 1986

Dynamics of vector spin glasses with random anisotropy
journal, June 1985

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

Magnetocaloric investigation of (H, T) phase diagram of CuMn spin glass
journal, January 1982

Dynamics of Cu-Mn spin-glass films
journal, July 1989

Grain size effect on the magnetic cluster-glass properties of La _0.88 Sr _0.12 CoO ₃
journal, February 2010

Low temperature cluster glass behavior in Nd ₅ Ge ₃
journal, November 2011

Spin-glass behavior in Ni-doped La $_{1.85}$ Sr $_{0.15}$ CuO $_{4}$
journal, July 2011

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

Three-dimensional Heisenberg spin-glass behavior in SrFe $_{0.90}$ Co $_{0.10}$ O $_{3.0}$
journal, August 2012

Cluster spin-glass behavior and memory effect in ${Cr}_{0.5} {Fe}_{0.5} Ga$
journal, October 2018

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

Evidence for a phase transition in the spin glass ${Eu}_{0.4}$ ${Sr}_{0.6}$ S from dynamic susceptibility measurements
journal, July 1987

Spin glass behavior in frustrated quantum spin system CuAl ₂ O ₄ with a possible orbital liquid state
journal, February 2017

Dynamic spin fluctuations in the frustrated $A$ -site spinel $Cu {Al}_{2} O_{4}$
journal, July 2020

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

Ferroelectricity in spiral short-range-ordered magnetic state of spinel ${MnCr}_{2} O_{4}$ : Significance of topological frustration and magnetoelastic coupling
journal, November 2014

Critical slowing down in spin glasses and other glasses: Fulcher versus power law
journal, July 1985

Transition from a paramagnetic metallic to a cluster glass metallic state in electron-doped perovskite manganites
journal, August 1998

Scaling of Nonlinear Susceptibility in MnCu and GdAl Spin-Glasses
journal, December 1981

Spin freezing in the spin-liquid compound ${FeAl}_{2} O_{4}$
journal, February 2015

Non-Mean-Field Interpretation of the Irreversibility Line in Spin-Glasses
journal, October 1983

Local order and frustration in the geometrically frustrated spinels ${Cd}_{1 - x} {Zn}_{x} V_{2} O_{4}$
journal, July 2006

Ordering and Antiferromagnetism in Ferrites
journal, May 1956

Critical Properties of a Random-Anisotropy System $a - DyNi$ : A New Universality Class in Disordered Systems?
journal, September 1986

Dynamic scaling in the Eu 0.4 Sr 0.6 S spin-glass
journal, December 1984

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

Dynamic susceptibility measurements at the spin-glass transition in the Zn _{1− x} Mn _x In ₂ Se ₄ semiconductor
journal, September 2007