Single-ion properties of the Seff = 12 XY antiferromagnetic pyrochlores NaA'Co2F7 ( A'=Ca2+, Sr2+ )

Ross, Kathryn A.; Brown, J. M.; Cava, R. J.; Krizan, J. W.; Nagler, Stephen E.; Rodriguez-Rivera, J. A.; Stone, Matthew B.

doi:10.1103/PhysRevB.95.144414

Title: Single-ion properties of the $S_{eff}$ = $\frac{1}{2}$ XY antiferromagnetic pyrochlores $Na A^{'} {Co}_{2} F_{7}$ ( $A^{'} = {Ca}^{2 +}, {Sr}^{2 +}$ )

Abstract

The antiferromagnetic pyrochlore material NaCaCo₂F₇ is a thermal spin liquid over a broad temperature range (≈140 K down to T_F=2.4 K), in which magnetic correlations between Co²⁺ dipole moments explore a continuous manifold of antiferromagnetic XY states. The thermal spin liquid is interrupted by spin freezing at a temperature that is ~2% of the mean-field interaction strength, leading to short-range static XY clusters with distinctive relaxation dynamics. Here we report the low-energy inelastic neutron scattering response from the related compound NaSrCo₂F₇, confirming that it hosts the same static and dynamic spin correlations as NaCaCo₂F₇. We then present the single-ion levels of Co²⁺ in these materials as measured by inelastic neutron scattering. An intermediate spin-orbit coupling model applied to an ensemble of trigonally distorted octahedral crystal fields accounts for the observed transitions. The single-ion ground state of Co²⁺ is a Kramers doublet with a strongly XY-like g tensor (gxy/gz~3). The local disorder inherent from the mixed pyrochlore A sites (Na⁺/Ca²⁺ and Na⁺/Sr²⁺) is evident in these measurements as exaggerated broadening of some of the levels. A simple model that reproduces the salient features of the single-ion spectrum produces approximately 8.4% and 4.1% variation in the z and xy components of themore »« less

Authors:

Ross, Kathryn A. ^[1]; Brown, J. M. ^[2]; Cava, R. J. ^[3]; Krizan, J. W. ^[3];

^[4]; Rodriguez-Rivera, J. A. ^[5];

^[4]

Colorado State Univ., Fort Collins, CO (United States); Canadian Institute for Advanced Research, Toronto, ON (Canada)
Colorado State Univ., Fort Collins, CO (United States)
Princeton Univ., Princeton, NJ (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States); Univ. of Maryland, College Park, MD (United States)

Publication Date:: 2017-04-13

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

Sponsoring Org.:: USDOE

OSTI Identifier:: 1471947

Alternate Identifier(s):: OSTI ID: 1351673

Grant/Contract Number:: AC05-00OR22725; FG02-08ER46544

Resource Type:: Accepted Manuscript

Journal Name:: Physical Review B

Additional Journal Information:: Journal Volume: 95; Journal Issue: 14; 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; 36 MATERIALS SCIENCE

Citation Formats


                    Ross, Kathryn A., Brown, J. M., Cava, R. J., Krizan, J. W., Nagler, Stephen E., Rodriguez-Rivera, J. A., and Stone, Matthew B. Single-ion properties of the Seff = 12 XY antiferromagnetic pyrochlores NaA'Co2F7 ( A'=Ca2+, Sr2+ ).  United States: N. p., 2017. 
Web.  doi:10.1103/PhysRevB.95.144414.

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                    Ross, Kathryn A., Brown, J. M., Cava, R. J., Krizan, J. W., Nagler, Stephen E., Rodriguez-Rivera, J. A., & Stone, Matthew B. Single-ion properties of the Seff = 12 XY antiferromagnetic pyrochlores NaA'Co2F7 ( A'=Ca2+, Sr2+ ).  United States.  https://doi.org/10.1103/PhysRevB.95.144414

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                    Ross, Kathryn A., Brown, J. M., Cava, R. J., Krizan, J. W., Nagler, Stephen E., Rodriguez-Rivera, J. A., and Stone, Matthew B. Thu .  
"Single-ion properties of the Seff = 12 XY antiferromagnetic pyrochlores NaA'Co2F7 ( A'=Ca2+, Sr2+ )".  United States.  https://doi.org/10.1103/PhysRevB.95.144414.  https://www.osti.gov/servlets/purl/1471947.

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@article{osti_1471947,

  title        = {Single-ion properties of the Seff = 12 XY antiferromagnetic pyrochlores NaA'Co2F7 ( A'=Ca2+, Sr2+ )},

  author       = {Ross, Kathryn A. and Brown, J. M. and Cava, R. J. and Krizan, J. W. and Nagler, Stephen E. and Rodriguez-Rivera, J. A. and Stone, Matthew B.},

  abstractNote = {The antiferromagnetic pyrochlore material NaCaCo2F7 is a thermal spin liquid over a broad temperature range (≈140 K down to TF=2.4 K), in which magnetic correlations between Co2+ dipole moments explore a continuous manifold of antiferromagnetic XY states. The thermal spin liquid is interrupted by spin freezing at a temperature that is ~2% of the mean-field interaction strength, leading to short-range static XY clusters with distinctive relaxation dynamics. Here we report the low-energy inelastic neutron scattering response from the related compound NaSrCo2F7, confirming that it hosts the same static and dynamic spin correlations as NaCaCo2F7. We then present the single-ion levels of Co2+ in these materials as measured by inelastic neutron scattering. An intermediate spin-orbit coupling model applied to an ensemble of trigonally distorted octahedral crystal fields accounts for the observed transitions. The single-ion ground state of Co2+ is a Kramers doublet with a strongly XY-like g tensor (gxy/gz~3). The local disorder inherent from the mixed pyrochlore A sites (Na+/Ca2+ and Na+/Sr2+) is evident in these measurements as exaggerated broadening of some of the levels. A simple model that reproduces the salient features of the single-ion spectrum produces approximately 8.4% and 4.1% variation in the z and xy components of the g tensor, respectively. In conclusion, this study confirms that an Seff = 1/2 model with XY antiferromagnetic exchange and weak exchange disorder serves as a basic starting point in understanding the low-temperature magnetic behavior of these strongly frustrated magnets.},

  doi          = {10.1103/PhysRevB.95.144414},

  journal      = {Physical Review B},

  number       = 14,

  volume       = 95,

  place        = {United States},

  year         = {2017},

  month        = {4}

}

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In this paper, we report inelastic neutron scattering experiments in Ca₂Y₂Cu₅O₁₀ and map out the full one-magnon dispersion which extends up to a record value of 53 meV for frustrated ferromagnetic (FM) edge-sharing CuO₂ chain (FFESC) cuprates. A homogeneous spin-1/2 chain model with a FM nearest-neighbor (NN), an antiferromagnetic (AFM) next-nearest-neighbor (NNN) inchain, and two diagonal AFM interchain couplings (ICs) analyzed within linear spin-wave theory (LSWT) reproduces well the observed strong dispersion along the chains and a weak one perpendicularly. The ratio α=|J_a2/J_a1| of the FM NN and the AFM NNN couplings is found as ~0.23, close to the critical point α_c=1/4 which separates ferromagnetically and antiferromagnetically correlated spiral magnetic ground states in single chains, whereas α_c>0.25 for coupled chains is considerably upshifted even for relatively weak IC. Although the measured dispersion can be described by homogeneous LSWT, the scattering intensity appears to be considerably reduced at ~11.5 and ~28 meV. The gaplike feature at 11.5 meV is attributed to magnon-phonon coupling whereas based on density matrix renormalization group simulations of the dynamical structure factor the gap at 28 meV is considered to stem partly from quantum effects due to the AFM IC. Another contribution to that gap is ascribed to the intrinsic superstructure from the distorting incommensurate pattern of CaY cationic chains adjacent to the CuO₂ ones. It gives rise to nonequivalent CuO₄ units and Cu-O-Cu bond angles Φ and a resulting distribution of all exchange integrals. The J's fitted by homogeneous LSWT are regarded as average values. The record value of the FM NN integral J₁=24 meV among FFESC cuprates can be explained by a nonuniversal Φ(≠90°) and Cu-O bond length dependent anisotropic mean direct FM Cu-O exchangemore »« less
Cited by 3
https://doi.org/10.1103/PhysRevB.100.104415

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Highly anisotropic exchange interactions of $j_{eff} = \frac{1}{2}$ iridium moments on the fcc lattice in ${La}_{2} B {IrO}_{6} (B = Mg, Zn)$

Journal Article Aczel, A. A. ; Cook, A. M. ; Williams, T. J. ; ... - Physical Review B

Here we have performed inelastic neutron scattering (INS) experiments to investigate the magnetic excitations in the weakly distorted face-centered-cubic (fcc) iridate double perovskites Lamore »« less
Cited by 6
https://doi.org/10.1103/PhysRevB.93.214426

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Title: Single-ion properties of the S eff = 1 2 XY antiferromagnetic pyrochlores Na A ' Co 2 F 7 ( A ' = Ca 2 + , Sr 2 + )

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Matrix Elements and Operator Equivalents Connected with the Magnetic Properties of Rare Earth Ions journal, March 1952

Order by Quantum Disorder in Er 2 Ti 2 O 7 journal, October 2012

Order from structural disorder in the X Y pyrochlore antiferromagnet Er 2 Ti 2 O 7 journal, September 2014

Mantid—Data analysis and visualization package for neutron scattering and μ SR experiments journal, November 2014

Spin Ice, Fractionalization, and Topological Order journal, March 2012

Quantum Order by Disorder and Accidental Soft Mode in Er 2 Ti 2 O 7 journal, August 2012

Revised effective ionic radii and systematic studies of interatomic distances in halides and chalcogenides journal, September 1976

Er 2 Ti 2 O 7 : Evidence of quantum order by disorder in a frustrated antiferromagnet journal, July 2003

Introduction to the Theory of Thermal Neutron Scattering book, May 2012

Antiferromagnetic order in the pyrochlores R 2 Ge 2 O 7 ( R = Er , Yb ) journal, October 2015

Order induced by dilution in pyrochlore XY antiferromagnets journal, February 2015

Crystal structure and vibrational spectrum of the NaCaMg2F7 pyrochlore journal, August 2004

Magnetic dilution and domain selection in the X Y pyrochlore antiferromagnet Er 2 Ti 2 O 7 journal, August 2016

Magnetic Properties of Co Cl 2 and Ni Cl 2 journal, July 1963

Phase transition and thermal order-by-disorder in the pyrochlore antiferromagnet Er 2 Ti 2 O 7 : A high-temperature series expansion study journal, December 2013

Experimental realization of a quantum breathing pyrochlore antiferromagnet journal, August 2014

Spin Waves and Quantum Criticality in the Frustrated X Y Pyrochlore Antiferromagnet Er 2 Ti 2 O 7 journal, October 2008

NaSrCo 2 F 7 , a Co 2+ pyrochlore antiferromagnet journal, July 2015

Order by disorder or energetic selection of the ground state in the X Y pyrochlore antiferromagnet Er 2 Ti 2 O 7 : An inelastic neutron scattering study journal, August 2014

Molecular spin-orbit excitations in the J eff = 1 2 frustrated spinel GeCo 2 O 4 journal, August 2011

Symmetry and light stuffing of H o 2 T i 2 O 7 , E r 2 T i 2 O 7 , and Y b 2 T i 2 O 7 characterized by synchrotron x-ray diffraction journal, July 2015

ISODISPLACE : a web-based tool for exploring structural distortions journal, July 2006

Theory of multiple-phase competition in pyrochlore magnets with anisotropic exchange with application to Yb 2 Ti 2 O 7 , Er 2 Ti 2 O 7 , and Er 2 Sn 2 O 7 journal, March 2017

Soft modes in the easy plane pyrochlore antiferromagnet journal, March 2004

High-pressure synthesis and characterization of the effective pseudospin S = 1 / 2 XY pyrochlores R 2 P t 2 O 7 ( R = Er , Yb ) journal, January 2016

Ground state phase diagram of generic X Y pyrochlore magnets with quantum fluctuations journal, October 2013

DAVE: A Comprehensive Software Suite for the Reduction, Visualization, and Analysis of Low Energy Neutron Spectroscopic Data journal, November 2009

Magnetic pyrochlore oxides journal, January 2010

Short-range magnetic order in the frustrated pyrochlore antiferromagnet CsNiCrF 6 journal, November 1997

Neutron spectroscopic study of crystal-field excitations and the effect of the crystal field on dipolar magnetism in Li R F 4 ( R = Gd , Ho, Er, Tm, and Yb) journal, October 2015

Order by disorder in an anisotropic pyrochlore lattice antiferromagnet journal, May 1994

NaCaN i 2 F 7 : A frustrated high-temperature pyrochlore antiferromagnet with S = 1 N i 2 + journal, July 2015

Order-by-disorder in the X Y pyrochlore antiferromagnet journal, January 2014

Quantum Excitations in Quantum Spin Ice journal, October 2011

MACS—a new high intensity cold neutron spectrometer at NIST journal, January 2008

Excitations in KCoF 3 . II. Theoretical journal, October 1971

Long-range order and spin-liquid states of polycrystalline Tb 2 + x Ti 2 − x O 7 + y journal, February 2013

Heat-capacity measurements on rare-earth double oxides R2M2O7 journal, September 1969

SEQUOIA: A fine resolution chopper spectrometer at the SNS journal, November 2006

Lightly stuffed pyrochlore structure of single-crystalline Yb 2 Ti 2 O 7 grown by the optical floating zone technique journal, November 2012

Magnetic ordering in the XY pyrochlore antiferromagnet Er 2 Ti 2 O 7 : a spherical neutron polarimetry study journal, October 2007

Static and dynamic X Y -like short-range order in a frustrated magnet with exchange disorder journal, January 2016

NaCaCo 2 F 7 : A single-crystal high-temperature pyrochlore antiferromagnet journal, June 2014

Exchange mixing and soliton dynamics in the quantum spin chain CsCoCl 3 journal, December 1995

Theory of the Magnetic Properties of Ferrous and Cobaltous Oxides, I journal, February 1957

NaSrMn 2 F 7 , NaCaFe 2 F 7 , and NaSrFe 2 F 7 : novel single crystal pyrochlore antiferromagnets journal, November 2016

Magnetic frustration in the disordered pyrochlore Yb 2 GaSbO 7 journal, April 2011

Synthesis of new high-pressure pyrochlore phases journal, August 1968

Single-crystal versus polycrystalline samples of magnetically frustrated Yb 2 Ti 2 O 7 : Specific heat results journal, November 2011

Palmer-Chalker correlations in the X Y pyrochlore antiferromagnet Er 2 Sn 2 O 7 journal, October 2013

Neutron spectroscopic study of crystalline electric field excitations in stoichiometric and lightly stuffed Yb 2 Ti 2 O 7 journal, October 2015

Introduction to the Theory of Thermal Neutron Scattering journal, December 1979

Spin Ice, Fractionalization and Topological Order text, January 2011

Order Induced by Dilution in Pyrochlore XY Antiferromagnets text, January 2014

Order by Disorder and Energetic Selection of the Ground State in the XY Pyrochlore Antiferromagnet Er2Ti2O7. An Inelastic Neutron Scattering Study text, January 2014

μ SR study of spin freezing and persistent spin dynamics in NaCaNi 2 F 7 journal, August 2018

Single crystal neutron and magnetic measurements of Rb 2 Mn 3 (VO 4 ) 2 CO 3 and K 2 Co 3 (VO 4 ) 2 CO 3 with mixed honeycomb and triangular magnetic lattices journal, January 2020

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Title: Single-ion properties of the $S_{eff}$ = $\frac{1}{2}$ XY antiferromagnetic pyrochlores $Na A^{'} {Co}_{2} F_{7}$ ( $A^{'} = {Ca}^{2 +}, {Sr}^{2 +}$ )

Matrix Elements and Operator Equivalents Connected with the Magnetic Properties of Rare Earth Ions
journal, March 1952

Order by Quantum Disorder in ${Er}_{2} {Ti}_{2} O_{7}$
journal, October 2012

Order from structural disorder in the $X Y$ pyrochlore antiferromagnet ${Er}_{2} {Ti}_{2} O_{7}$
journal, September 2014

Mantid—Data analysis and visualization package for neutron scattering and $μ$ SR experiments
journal, November 2014

Spin Ice, Fractionalization, and Topological Order
journal, March 2012

Quantum Order by Disorder and Accidental Soft Mode in ${Er}_{2} {Ti}_{2} O_{7}$
journal, August 2012

Revised effective ionic radii and systematic studies of interatomic distances in halides and chalcogenides
journal, September 1976

${Er}_{2} {Ti}_{2} O_{7} :$ Evidence of quantum order by disorder in a frustrated antiferromagnet
journal, July 2003

Introduction to the Theory of Thermal Neutron Scattering
book, May 2012

Antiferromagnetic order in the pyrochlores $R_{2} {Ge}_{2} O_{7} (R = Er, Yb)$
journal, October 2015

Order induced by dilution in pyrochlore XY antiferromagnets
journal, February 2015

Crystal structure and vibrational spectrum of the NaCaMg2F7 pyrochlore
journal, August 2004

Magnetic dilution and domain selection in the $X Y$ pyrochlore antiferromagnet ${Er}_{2} {Ti}_{2} O_{7}$
journal, August 2016

Magnetic Properties of Co ${Cl}_{2}$ and Ni ${Cl}_{2}$
journal, July 1963

Phase transition and thermal order-by-disorder in the pyrochlore antiferromagnet Er $_{2}$ Ti $_{2}$ O $_{7}$ : A high-temperature series expansion study
journal, December 2013

Experimental realization of a quantum breathing pyrochlore antiferromagnet
journal, August 2014

Spin Waves and Quantum Criticality in the Frustrated $X Y$ Pyrochlore Antiferromagnet ${Er}_{2} {Ti}_{2} O_{7}$
journal, October 2008

NaSrCo ₂ F ₇ , a Co ²⁺ pyrochlore antiferromagnet
journal, July 2015

Order by disorder or energetic selection of the ground state in the $X Y$ pyrochlore antiferromagnet ${Er}_{2} {Ti}_{2} O_{7}$ : An inelastic neutron scattering study
journal, August 2014

Molecular spin-orbit excitations in the $J_{eff}$ = $\frac{1}{2}$ frustrated spinel GeCo $_{2}$ O $_{4}$
journal, August 2011

Symmetry and light stuffing of $H o_{2} T i_{2} O_{7}, E r_{2} T i_{2} O_{7}$ , and $Y b_{2} T i_{2} O_{7}$ characterized by synchrotron x-ray diffraction
journal, July 2015

ISODISPLACE : a web-based tool for exploring structural distortions
journal, July 2006

Theory of multiple-phase competition in pyrochlore magnets with anisotropic exchange with application to ${Yb}_{2} {Ti}_{2} O_{7}, {Er}_{2} {Ti}_{2} O_{7}$ , and ${Er}_{2} {Sn}_{2} O_{7}$
journal, March 2017

Soft modes in the easy plane pyrochlore antiferromagnet
journal, March 2004

High-pressure synthesis and characterization of the effective pseudospin $S = 1 / 2$ XY pyrochlores $R_{2} P t_{2} O_{7} (R = Er, Yb)$
journal, January 2016

Ground state phase diagram of generic $X Y$ pyrochlore magnets with quantum fluctuations
journal, October 2013

DAVE: A Comprehensive Software Suite for the Reduction, Visualization, and Analysis of Low Energy Neutron Spectroscopic Data
journal, November 2009

Magnetic pyrochlore oxides
journal, January 2010

Short-range magnetic order in the frustrated pyrochlore antiferromagnet ${CsNiCrF}_{6}$
journal, November 1997

Neutron spectroscopic study of crystal-field excitations and the effect of the crystal field on dipolar magnetism in $Li R F_{4}$ ( $R = Gd$ , Ho, Er, Tm, and Yb)
journal, October 2015

Order by disorder in an anisotropic pyrochlore lattice antiferromagnet
journal, May 1994

$NaCaN i_{2} F_{7}$ : A frustrated high-temperature pyrochlore antiferromagnet with $S = 1 N i^{2 +}$
journal, July 2015

Order-by-disorder in the $X Y$ pyrochlore antiferromagnet
journal, January 2014

Quantum Excitations in Quantum Spin Ice
journal, October 2011

MACS—a new high intensity cold neutron spectrometer at NIST
journal, January 2008

Excitations in KCoF ₃ . II. Theoretical
journal, October 1971

Long-range order and spin-liquid states of polycrystalline Tb $_{2 + x}$ Ti $_{2 - x}$ O $_{7 + y}$
journal, February 2013

Heat-capacity measurements on rare-earth double oxides R2M2O7
journal, September 1969

SEQUOIA: A fine resolution chopper spectrometer at the SNS
journal, November 2006

Lightly stuffed pyrochlore structure of single-crystalline Yb $_{2}$ Ti $_{2}$ O $_{7}$ grown by the optical floating zone technique
journal, November 2012

Magnetic ordering in the XY pyrochlore antiferromagnet Er ₂ Ti ₂ O ₇ : a spherical neutron polarimetry study
journal, October 2007

Static and dynamic $X Y$ -like short-range order in a frustrated magnet with exchange disorder
journal, January 2016

${NaCaCo}_{2} F_{7}$ : A single-crystal high-temperature pyrochlore antiferromagnet
journal, June 2014

Exchange mixing and soliton dynamics in the quantum spin chain ${CsCoCl}_{3}$
journal, December 1995

Theory of the Magnetic Properties of Ferrous and Cobaltous Oxides, I
journal, February 1957

NaSrMn ₂ F ₇ , NaCaFe ₂ F ₇ , and NaSrFe ₂ F ₇ : novel single crystal pyrochlore antiferromagnets
journal, November 2016

Magnetic frustration in the disordered pyrochlore Yb ₂ GaSbO ₇
journal, April 2011

Synthesis of new high-pressure pyrochlore phases
journal, August 1968

Single-crystal versus polycrystalline samples of magnetically frustrated Yb $_{2}$ Ti $_{2}$ O $_{7}$ : Specific heat results
journal, November 2011

Palmer-Chalker correlations in the $X Y$ pyrochlore antiferromagnet Er $_{2}$ Sn $_{2}$ O $_{7}$
journal, October 2013

Neutron spectroscopic study of crystalline electric field excitations in stoichiometric and lightly stuffed ${Yb}_{2} {Ti}_{2} O_{7}$
journal, October 2015

Introduction to the Theory of Thermal Neutron Scattering
journal, December 1979

Spin Ice, Fractionalization and Topological Order
text, January 2011

Order Induced by Dilution in Pyrochlore XY Antiferromagnets
text, January 2014

Order by Disorder and Energetic Selection of the Ground State in the XY Pyrochlore Antiferromagnet Er2Ti2O7. An Inelastic Neutron Scattering Study
text, January 2014

μ SR study of spin freezing and persistent spin dynamics in NaCaNi ₂ F ₇
journal, August 2018

Single crystal neutron and magnetic measurements of Rb ₂ Mn ₃ (VO ₄ ) ₂ CO ₃ and K ₂ Co ₃ (VO ₄ ) ₂ CO ₃ with mixed honeycomb and triangular magnetic lattices
journal, January 2020

Pseudospin exchange interactions in $d^{7}$ cobalt compounds: Possible realization of the Kitaev model
journal, January 2018

Intrinsic transverse field in frustrated quantum Ising magnets: Physical origin and quantum effects
journal, December 2019

Competing Spin Liquids and Hidden Spin-Nematic Order in Spin Ice with Frustrated Transverse Exchange
journal, December 2017