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 $Na A^{'} {Co}_{2} F_{7}$ ( $A^{'} = {Ca}^{2 +}, {Sr}^{2 +}$ )

Journal Article · Thu Apr 13 00:00:00 EDT 2017 · Physical Review B

DOI:https://doi.org/10.1103/PhysRevB.95.144414· OSTI ID:1471947

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)

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 the g tensor, respectively. In conclusion, this study confirms that an S_eff = 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.

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Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE

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

OSTI ID:: 1471947

Alternate ID(s):: OSTI ID: 1351673

Journal Information:: Physical Review B, Vol. 95, Issue 14; ISSN 2469-9950

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 39 works

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References (54)

Matrix Elements and Operator Equivalents Connected with the Magnetic Properties of Rare Earth Ions Stevens, K. W. H. Proceedings of the Physical Society. Section A, Vol. 65, Issue 3 https://doi.org/10.1088/0370-1298/65/3/308	journal	March 1952
Order by Quantum Disorder in ${Er}_{2} {Ti}_{2} O_{7}$ Savary, Lucile; Ross, Kate A.; Gaulin, Bruce D. Physical Review Letters, Vol. 109, Issue 16 https://doi.org/10.1103/PhysRevLett.109.167201	journal	October 2012
Order from structural disorder in the $X Y$ pyrochlore antiferromagnet ${Er}_{2} {Ti}_{2} O_{7}$ Maryasin, V. S.; Zhitomirsky, M. E. Physical Review B, Vol. 90, Issue 9 https://doi.org/10.1103/PhysRevB.90.094412	journal	September 2014
Mantid—Data analysis and visualization package for neutron scattering and $μ$ SR experiments Arnold, O.; Bilheux, J. C.; Borreguero, J. M. Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment, Vol. 764 https://doi.org/10.1016/j.nima.2014.07.029	journal	November 2014
Spin Ice, Fractionalization, and Topological Order Castelnovo, C.; Moessner, R.; Sondhi, S. L. Annual Review of Condensed Matter Physics, Vol. 3, Issue 1 https://doi.org/10.1146/annurev-conmatphys-020911-125058	journal	March 2012
Quantum Order by Disorder and Accidental Soft Mode in ${Er}_{2} {Ti}_{2} O_{7}$ Zhitomirsky, M. E.; Gvozdikova, M. V.; Holdsworth, P. C. W. Physical Review Letters, Vol. 109, Issue 7 https://doi.org/10.1103/PhysRevLett.109.077204	journal	August 2012
Revised effective ionic radii and systematic studies of interatomic distances in halides and chalcogenides Shannon, R. D. Acta Crystallographica Section A, Vol. 32, Issue 5, p. 751-767 https://doi.org/10.1107/S0567739476001551	journal	September 1976
${Er}_{2} {Ti}_{2} O_{7} :$ Evidence of quantum order by disorder in a frustrated antiferromagnet Champion, J. D. M.; Harris, M. J.; Holdsworth, P. C. W. Physical Review B, Vol. 68, Issue 2 https://doi.org/10.1103/PhysRevB.68.020401	journal	July 2003
Introduction to the Theory of Thermal Neutron Scattering Squires, G. L. https://doi.org/10.1017/CBO9781139107808	book	May 2012
Antiferromagnetic order in the pyrochlores $R_{2} {Ge}_{2} O_{7} (R = Er, Yb)$ Dun, Z. L.; Li, X.; Freitas, R. S. Physical Review B, Vol. 92, Issue 14 https://doi.org/10.1103/PhysRevB.92.140407	journal	October 2015
Order induced by dilution in pyrochlore XY antiferromagnets Andreanov, A.; McClarty, P. A. Physical Review B, Vol. 91, Issue 6 https://doi.org/10.1103/PhysRevB.91.064401	journal	February 2015
Crystal structure and vibrational spectrum of the NaCaMg2F7 pyrochlore Oliveira, E. A.; Guedes, I.; Ayala, A. P. Journal of Solid State Chemistry, Vol. 177, Issue 8 https://doi.org/10.1016/j.jssc.2004.04.055	journal	August 2004
Magnetic dilution and domain selection in the $X Y$ pyrochlore antiferromagnet ${Er}_{2} {Ti}_{2} O_{7}$ Gaudet, J.; Hallas, A. M.; Maharaj, D. D. Physical Review B, Vol. 94, Issue 6 https://doi.org/10.1103/PhysRevB.94.060407	journal	August 2016
Magnetic Properties of Co ${Cl}_{2}$ and Ni ${Cl}_{2}$ Lines, M. E. Physical Review, Vol. 131, Issue 2 https://doi.org/10.1103/PhysRev.131.546	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 Oitmaa, J.; Singh, R. R. P.; Javanparast, B. Physical Review B, Vol. 88, Issue 22 https://doi.org/10.1103/PhysRevB.88.220404	journal	December 2013
Experimental realization of a quantum breathing pyrochlore antiferromagnet Kimura, K.; Nakatsuji, S.; Kimura, T. Physical Review B, Vol. 90, Issue 6 https://doi.org/10.1103/PhysRevB.90.060414	journal	August 2014
Spin Waves and Quantum Criticality in the Frustrated $X Y$ Pyrochlore Antiferromagnet ${Er}_{2} {Ti}_{2} O_{7}$ Ruff, J. P. C.; Clancy, J. P.; Bourque, A. Physical Review Letters, Vol. 101, Issue 14 https://doi.org/10.1103/PhysRevLett.101.147205	journal	October 2008
NaSrCo ₂ F ₇ , a Co ²⁺ pyrochlore antiferromagnet Krizan, J. W.; Cava, R. J. Journal of Physics: Condensed Matter, Vol. 27, Issue 29 https://doi.org/10.1088/0953-8984/27/29/296002	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 Petit, Sylvain; Robert, Julien; Guitteny, Solène Physical Review B, Vol. 90, Issue 6 https://doi.org/10.1103/PhysRevB.90.060410	journal	August 2014
Molecular spin-orbit excitations in the $J_{eff}$ = $\frac{1}{2}$ frustrated spinel GeCo $_{2}$ O $_{4}$ Tomiyasu, K.; Crawford, M. K.; Adroja, D. T. Physical Review B, Vol. 84, Issue 5 https://doi.org/10.1103/PhysRevB.84.054405	journal	August 2011
ISODISPLACE : a web-based tool for exploring structural distortions Campbell, Branton J.; Stokes, Harold T.; Tanner, David E. Journal of Applied Crystallography, Vol. 39, Issue 4 https://doi.org/10.1107/S0021889806014075	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 ${Er}_{2} {Sn}_{2} O_{7}$ Yan, Han; Benton, Owen; Jaubert, Ludovic Physical Review B, Vol. 95, Issue 9 https://doi.org/10.1103/PhysRevB.95.094422	journal	March 2017
Soft modes in the easy plane pyrochlore antiferromagnet Champion, J. D. M.; Holdsworth, P. C. W. Journal of Physics: Condensed Matter, Vol. 16, Issue 11 https://doi.org/10.1088/0953-8984/16/11/013	journal	March 2004
High-pressure synthesis and characterization of the effective pseudospin $S = 1 / 2$ XY pyrochlores $R_{2} P t_{2} O_{7} (R = Er, Yb)$ Cai, Y. Q.; Cui, Q.; Li, X. Physical Review B, Vol. 93, Issue 1 https://doi.org/10.1103/PhysRevB.93.014443	journal	January 2016
Ground state phase diagram of generic $X Y$ pyrochlore magnets with quantum fluctuations Wong, Anson W. C.; Hao, Zhihao; Gingras, Michel J. P. Physical Review B, Vol. 88, Issue 14 https://doi.org/10.1103/PhysRevB.88.144402	journal	October 2013
DAVE: A Comprehensive Software Suite for the Reduction, Visualization, and Analysis of Low Energy Neutron Spectroscopic Data Azuah, Richard Tumanjong; Kneller, Larry R.; Qiu, Yiming Journal of Research of the National Institute of Standards and Technology, Vol. 114, Issue 6 https://doi.org/10.6028/jres.114.025	journal	November 2009
Magnetic pyrochlore oxides Gardner, Jason S.; Gingras, Michel J. P.; Greedan, John E. Reviews of Modern Physics, Vol. 82, Issue 1 https://doi.org/10.1103/RevModPhys.82.53	journal	January 2010
Short-range magnetic order in the frustrated pyrochlore antiferromagnet ${CsNiCrF}_{6}$ Zinkin, M. P.; Harris, M. J.; Zeiske, T. Physical Review B, Vol. 56, Issue 18 https://doi.org/10.1103/PhysRevB.56.11786	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) Babkevich, P.; Finco, A.; Jeong, M. Physical Review B, Vol. 92, Issue 14 https://doi.org/10.1103/PhysRevB.92.144422	journal	October 2015
Order by disorder in an anisotropic pyrochlore lattice antiferromagnet Bramwell, S. T.; Gingras, M. J. P.; Reimers, J. N. Journal of Applied Physics, Vol. 75, Issue 10 https://doi.org/10.1063/1.355676	journal	May 1994
$NaCaN i_{2} F_{7}$ : A frustrated high-temperature pyrochlore antiferromagnet with $S = 1 N i^{2 +}$ Krizan, J. W.; Cava, R. J. Physical Review B, Vol. 92, Issue 1 https://doi.org/10.1103/PhysRevB.92.014406	journal	July 2015
Order-by-disorder in the $X Y$ pyrochlore antiferromagnet McClarty, Paul A.; Stasiak, Pawel; Gingras, Michel J. P. Physical Review B, Vol. 89, Issue 2 https://doi.org/10.1103/PhysRevB.89.024425	journal	January 2014
Quantum Excitations in Quantum Spin Ice Ross, Kate A.; Savary, Lucile; Gaulin, Bruce D. Physical Review X, Vol. 1, Issue 2 https://doi.org/10.1103/PhysRevX.1.021002	journal	October 2011
MACS—a new high intensity cold neutron spectrometer at NIST Rodriguez, J. A.; Adler, D. M.; Brand, P. C. Measurement Science and Technology, Vol. 19, Issue 3 https://doi.org/10.1088/0957-0233/19/3/034023	journal	January 2008
Excitations in KCoF ₃ . II. Theoretical Buyers, W. J. L.; Holden, T. M.; Svensson, E. C. Journal of Physics C: Solid State Physics, Vol. 4, Issue 14 https://doi.org/10.1088/0022-3719/4/14/028	journal	October 1971
Long-range order and spin-liquid states of polycrystalline Tb $_{2 + x}$ Ti $_{2 - x}$ O $_{7 + y}$ Taniguchi, T.; Kadowaki, H.; Takatsu, H. Physical Review B, Vol. 87, Issue 6 https://doi.org/10.1103/PhysRevB.87.060408	journal	February 2013
Heat-capacity measurements on rare-earth double oxides R2M2O7 Blöte, H. W. J.; Wielinga, R. F.; Huiskamp, W. J. Physica, Vol. 43, Issue 4 https://doi.org/10.1016/0031-8914(69)90187-6	journal	September 1969
SEQUOIA: A fine resolution chopper spectrometer at the SNS Granroth, G. E.; Vandergriff, D. H.; Nagler, S. E. Physica B: Condensed Matter, Vol. 385-386 https://doi.org/10.1016/j.physb.2006.05.379	journal	November 2006
Lightly stuffed pyrochlore structure of single-crystalline Yb $_{2}$ Ti $_{2}$ O $_{7}$ grown by the optical floating zone technique Ross, K. A.; Proffen, Th.; Dabkowska, H. A. Physical Review B, Vol. 86, Issue 17 https://doi.org/10.1103/PhysRevB.86.174424	journal	November 2012
Magnetic ordering in the XY pyrochlore antiferromagnet Er ₂ Ti ₂ O ₇ : a spherical neutron polarimetry study Poole, A.; Wills, A. S.; Lelièvre-Berna, E. Journal of Physics: Condensed Matter, Vol. 19, Issue 45 https://doi.org/10.1088/0953-8984/19/45/452201	journal	October 2007
Static and dynamic $X Y$ -like short-range order in a frustrated magnet with exchange disorder Ross, K. A.; Krizan, J. W.; Rodriguez-Rivera, J. A. Physical Review B, Vol. 93, Issue 1 https://doi.org/10.1103/PhysRevB.93.014433	journal	January 2016
${NaCaCo}_{2} F_{7}$ : A single-crystal high-temperature pyrochlore antiferromagnet Krizan, J. W.; Cava, R. J. Physical Review B, Vol. 89, Issue 21 https://doi.org/10.1103/PhysRevB.89.214401	journal	June 2014
Exchange mixing and soliton dynamics in the quantum spin chain ${CsCoCl}_{3}$ Goff, J. P.; Tennant, D. A.; Nagler, S. E. Physical Review B, Vol. 52, Issue 22 https://doi.org/10.1103/PhysRevB.52.15992	journal	December 1995
Theory of the Magnetic Properties of Ferrous and Cobaltous Oxides, I Kanamori, Junjiro Progress of Theoretical Physics, Vol. 17, Issue 2 https://doi.org/10.1143/PTP.17.177	journal	February 1957
Magnetic frustration in the disordered pyrochlore Yb ₂ GaSbO ₇ Hodges, J. A.; de Réotier, P. Dalmas; Yaouanc, A. Journal of Physics: Condensed Matter, Vol. 23, Issue 16 https://doi.org/10.1088/0953-8984/23/16/164217	journal	April 2011
Synthesis of new high-pressure pyrochlore phases Shannon, R. D.; Sleight, A. W. Inorganic Chemistry, Vol. 7, Issue 8 https://doi.org/10.1021/ic50066a038	journal	August 1968
Single-crystal versus polycrystalline samples of magnetically frustrated Yb $_{2}$ Ti $_{2}$ O $_{7}$ : Specific heat results Yaouanc, A.; Dalmas de Réotier, P.; Marin, C. Physical Review B, Vol. 84, Issue 17 https://doi.org/10.1103/PhysRevB.84.172408	journal	November 2011
Palmer-Chalker correlations in the $X Y$ pyrochlore antiferromagnet Er $_{2}$ Sn $_{2}$ O $_{7}$ Guitteny, Solene; Petit, Sylvain; Lhotel, Elsa Physical Review B, Vol. 88, Issue 13 https://doi.org/10.1103/PhysRevB.88.134408	journal	October 2013
Neutron spectroscopic study of crystalline electric field excitations in stoichiometric and lightly stuffed ${Yb}_{2} {Ti}_{2} O_{7}$ Gaudet, J.; Maharaj, D. D.; Sala, G. Physical Review B, Vol. 92, Issue 13 https://doi.org/10.1103/PhysRevB.92.134420	journal	October 2015
Point-Charge Calculations of Energy Levels of Magnetic Ions in Crystalline Electric Fields Hutchings, Michael T. Solid State Physics https://doi.org/10.1016/S0081-1947(08)60517-2	book	January 1964
Introduction to the Theory of Thermal Neutron Scattering Bacon, G. E. Physics Bulletin, Vol. 30, Issue 12 https://doi.org/10.1088/0031-9112/30/12/044	journal	December 1979
Spin Ice, Fractionalization and Topological Order Castelnovo, C.; Moessner, R.; Sondhi, S. L. arXiv https://doi.org/10.48550/arxiv.1112.3793	text	January 2011
Order Induced by Dilution in Pyrochlore XY Antiferromagnets Andreanov, A.; McClarty, P. A. arXiv https://doi.org/10.48550/arxiv.1408.7119	text	January 2014
Order by Disorder and Energetic Selection of the Ground State in the XY Pyrochlore Antiferromagnet Er2Ti2O7. An Inelastic Neutron Scattering Study Petit, S.; Robert, J.; Guitteny, S. arXiv https://doi.org/10.48550/arxiv.1410.6198	text	January 2014

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