Spin gaps in the ordered states of La2LiXO6(X=Ru,Os) and their relation to the distortion of the cubic double perovskite structure in 4d3 and 5d3 magnets

Maharaj, D. D.; Sala, G.; Marjerrison, C. A.; Stone, M. B.; Greedan, J. E.; Gaulin, B. D.

doi:10.1103/PhysRevB.98.104434

Title: Spin gaps in the ordered states of ${La}_{2} Li X O_{6} (X = Ru, Os)$ and their relation to the distortion of the cubic double perovskite structure in $4 d^{3}$ and $5 d^{3}$ magnets

Journal Article · Fri Sep 28 00:00:00 EDT 2018 · Physical Review B

DOI:https://doi.org/10.1103/PhysRevB.98.104434· OSTI ID:1493992

Maharaj, D. D. ^[1]; Sala, G. ^[2]; Marjerrison, C. A. ^[1]; Stone, M. B. ^[3]; Greedan, J. E. ^[1]; Gaulin, B. D. ^[4]

McMaster Univ., Hamilton, ON (Canada)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); McMaster Univ., Hamilton, ON (Canada)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
McMaster Univ., Hamilton, ON (Canada); Canadian Inst. for Advanced Research, Toronto, ON (Canada)

Time-of-flight inelastic neutron scattering measurements have been carried out on polycrystalline samples of the 4d³ and 5d³ double pervoskite antiferromagnets La₂LiRuO₆ and La₂LiOsO₆. These reveal the development of an inelastic spin gap in La₂LiRuO₆ and La₂LiOsO₆ of ~1.8(8) and 6(1) meV, below their respective ordering temperatures TN, ~23.8 and 30 K. The bandwidths of the spin excitations are shown to be ~5.7(9)and12(1)meV, respectively, at low temperatures. Spin gaps are surprising in such magnets as the t_2g levels of Ru⁵⁺ or Os⁵⁺ are expected to be half-filled, resulting in an anticipated orbital singlet for both materials. We compare these results in monoclinic double perovskites La₂LiRuO₆ and La₂LiOsO₆ with those in cubic Ba₂YRuO₆ and Ba₂YOsO₆ as well as with those in other monoclinic La₂NaRuO₆,La₂NaOsO₆, and Sr₂ScOsO₆ and model the inelastic magnetic scattering with linear spin-wave theory using minimal anisotropic exchange interactions. We discuss the possible role of the distortion of the face-centered-cubic double perovskite structure on the spin gap formation and geometric frustration in these materials and show that T_N scales with the top of the spin-wave band in all members of these families that display long-range order.

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

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

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1493992

Alternate ID(s):: OSTI ID: 1474770

Journal Information:: Physical Review B, Vol. 98, Issue 10; ISSN 2469-9950

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 7 works

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References (32)

Radial integrals for the magnetic form factor of 5 d transition elements Kobayashi, Kohjiro; Nagao, Tatsuya; Ito, Masahisa Acta Crystallographica Section A Foundations of Crystallography, Vol. 67, Issue 5 https://doi.org/10.1107/S010876731102633X	journal	August 2011
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
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
Triplet and in-gap magnetic states in the ground state of the quantum frustrated fcc antiferromagnet Ba $_{2}$ YMoO $_{6}$ Carlo, J. P.; Clancy, J. P.; Aharen, T. Physical Review B, Vol. 84, Issue 10 https://doi.org/10.1103/PhysRevB.84.100404	journal	September 2011
Correlated Quantum Phenomena in the Strong Spin-Orbit Regime Witczak-Krempa, William; Chen, Gang; Kim, Yong Baek Annual Review of Condensed Matter Physics, Vol. 5, Issue 1 https://doi.org/10.1146/annurev-conmatphys-020911-125138	journal	March 2014
Systematic analysis of spectroscopic characteristics of heavy transition metal ions with 4dN and 5dN (N=1…10) electronic configurations in a free state Ma, C. -G.; Brik, M. G. Journal of Luminescence, Vol. 145 https://doi.org/10.1016/j.jlumin.2013.07.075	journal	January 2014
SEQUOIA: A Newly Operating Chopper Spectrometer at the SNS Granroth, G. E.; Kolesnikov, A. I.; Sherline, T. E. Journal of Physics: Conference Series, Vol. 251 https://doi.org/10.1088/1742-6596/251/1/012058	journal	November 2010
Active role of nonmagnetic cations in magnetic interactions for double-perovskite $S r_{2} B Os O_{6} (B = Y, In, Sc)$ Kanungo, Sudipta; Yan, Binghai; Felser, Claudia Physical Review B, Vol. 93, Issue 16 https://doi.org/10.1103/PhysRevB.93.161116	journal	April 2016
Exotic Magnetism on the Quasi-fcc Lattices of the $d^{3}$ Double Perovskites ${La}_{2} Na B^{'} O_{6}$ ( $B^{'} = Ru$ , Os) Aczel, A. A.; Baker, P. J.; Bugaris, D. E. Physical Review Letters, Vol. 112, Issue 11 https://doi.org/10.1103/PhysRevLett.112.117603	journal	March 2014
Magnetic order and electronic structure of the $5 d^{3}$ double perovskite ${Sr}_{2} {ScOsO}_{6}$ Taylor, A. E.; Morrow, R.; Singh, D. J. Physical Review B, Vol. 91, Issue 10 https://doi.org/10.1103/PhysRevB.91.100406	journal	March 2015
Frustrated fcc antiferromagnet ${Ba}_{2} {YOsO}_{6}$ : Structural characterization, magnetic properties, and neutron scattering studies Kermarrec, E.; Marjerrison, C. A.; Thompson, C. M. Physical Review B, Vol. 91, Issue 7 https://doi.org/10.1103/PhysRevB.91.075133	journal	February 2015
B-cation arrangements in double perovskites Anderson, M.; Greenwood, K.; Taylor, G. Progress in Solid State Chemistry, Vol. 22, Issue 3 https://doi.org/10.1016/0079-6786(93)90004-B	journal	January 1993
Magnetically Frustrated Double Perovskites: Synthesis, Structural Properties, and Magnetic Order of Sr ₂ B OsO ₆ ( B = Y, In, Sc) : Magnetically Frustrated Double Perovskites Sr Paul, Avijit Kumar; Sarapulova, Angelina; Adler, Peter Zeitschrift für anorganische und allgemeine Chemie, Vol. 641, Issue 2 https://doi.org/10.1002/zaac.201400590	journal	February 2015
Frustration by competing interactions in the highly distorted double perovskites La $_{2}$ Na $B^{'}$ O $_{6}$ ( $B^{'} = Ru$ , Os) Aczel, A. A.; Bugaris, D. E.; Li, L. Physical Review B, Vol. 87, Issue 1 https://doi.org/10.1103/PhysRevB.87.014435	journal	January 2013
Kitaev materials beyond iridates: Order by quantum disorder and Weyl magnons in rare-earth double perovskites Li, Fei-Ye; Li, Yao-Dong; Yu, Yue Physical Review B, Vol. 95, Issue 8 https://doi.org/10.1103/PhysRevB.95.085132	journal	February 2017
Exotic phases induced by strong spin-orbit coupling in ordered double perovskites Chen, Gang; Pereira, Rodrigo; Balents, Leon Physical Review B, Vol. 82, Issue 17 https://doi.org/10.1103/PhysRevB.82.174440	journal	November 2010
Magnetic properties of the $S = \frac{3}{2}$ geometrically frustrated double perovskites ${La}_{2} {LiRuO}_{6}$ and ${Ba}_{2} {YRuO}_{6}$ Aharen, Tomoko; Greedan, John E.; Ning, Fanlong Physical Review B, Vol. 80, Issue 13 https://doi.org/10.1103/PhysRevB.80.134423	journal	October 2009
Frustrated magnetism in the double perovskite $L a_{2} LiOs O_{6}$ : A comparison with $L a_{2} LiRu O_{6}$ Thompson, C. M.; Marjerrison, C. A.; Sharma, A. Z. Physical Review B, Vol. 93, Issue 1 https://doi.org/10.1103/PhysRevB.93.014431	journal	January 2016
Long-range magnetic order in the 5 d ² double perovskite Ba ₂ CaOsO ₆ : comparison with spin-disordered Ba ₂ YReO ₆ Thompson, C. M.; Carlo, J. P.; Flacau, R. Journal of Physics: Condensed Matter, Vol. 26, Issue 30 https://doi.org/10.1088/0953-8984/26/30/306003	journal	July 2014
Magnetic properties of the geometrically frustrated $S = \frac{1}{2}$ antiferromagnets, ${La}_{2} {LiMoO}_{6}$ and ${Ba}_{2} {YMoO}_{6}$ , with the B-site ordered double perovskite structure: Evidence for a collective spin-singlet ground state Aharen, Tomoko; Greedan, John E.; Bridges, Craig A. Physical Review B, Vol. 81, Issue 22 https://doi.org/10.1103/PhysRevB.81.224409	journal	June 2010
Spin-orbit coupling controlled ground state in ${Sr}_{2} {ScOsO}_{6}$ Taylor, A. E.; Morrow, R.; Fishman, R. S. Physical Review B, Vol. 93, Issue 22 https://doi.org/10.1103/PhysRevB.93.220408	journal	June 2016
Phase-Sensitive Observation of a Spin-Orbital Mott State in Sr2IrO4 Kim, B. J.; Ohsumi, H.; Komesu, T. Science, Vol. 323, Issue 5919 https://doi.org/10.1126/science.1167106	journal	March 2009
Introduction to Frustrated Magnetism Lacroix, Claudine; Mendels, Philippe; Mila, Frédéric Springer Series in Solid-State Sciences https://doi.org/10.1007/978-3-642-10589-0	book	January 2011
${Ba}_{2} {YIrO}_{6}$ : A cubic double perovskite material with ${Ir}^{5 +}$ ions Dey, T.; Maljuk, A.; Efremov, D. V. Physical Review B, Vol. 93, Issue 1 https://doi.org/10.1103/PhysRevB.93.014434	journal	January 2016
Linear spin wave theory for single-Q incommensurate magnetic structures Toth, S.; Lake, B. Journal of Physics: Condensed Matter, Vol. 27, Issue 16 https://doi.org/10.1088/0953-8984/27/16/166002	journal	March 2015
Magnetic and Structural Studies of Sc Containing Ruthenate Double Perovskites A ₂ ScRuO ₆ ( A = Ba, Sr) Kayser, Paula; Injac, Sean; Ranjbar, Ben Inorganic Chemistry, Vol. 56, Issue 15 https://doi.org/10.1021/acs.inorgchem.7b00983	journal	July 2017
Structure and magnetic properties of the $S = 1$ geometrically frustrated double perovskites ${La}_{2} {LiReO}_{6}$ and ${Ba}_{2} {YReO}_{6}$ Aharen, Tomoko; Greedan, John E.; Bridges, Craig A. Physical Review B, Vol. 81, Issue 6 https://doi.org/10.1103/PhysRevB.81.064436	journal	February 2010
Spin gap and the nature of the 4 $d^{3}$ magnetic ground state in the frustrated fcc antiferromagnet Ba $_{2}$ YRuO $_{6}$ Carlo, J. P.; Clancy, J. P.; Fritsch, K. Physical Review B, Vol. 88, Issue 2 https://doi.org/10.1103/PhysRevB.88.024418	journal	July 2013
Spin-orbit coupling in $d^{2}$ ordered double perovskites Chen, Gang; Balents, Leon Physical Review B, Vol. 84, Issue 9 https://doi.org/10.1103/PhysRevB.84.094420	journal	September 2011
Correlated quantum phenomena in the strong spin-orbit regime Witczak-Krempa, William; Chen, Gang; Kim, Yong Baek arXiv https://doi.org/10.48550/arxiv.1305.2193	text	January 2013
Linear spin wave theory for single-Q incommensurate magnetic structures Toth, S.; Lake, B. arXiv https://doi.org/10.48550/arxiv.1402.6069	text	January 2014
Kitaev materials beyond iridates: order by quantum disorder and Weyl magnons in rare-earth double perovskites Li, Fei-Ye; Li, Yao-Dong; Yu, Yue arXiv https://doi.org/10.48550/arxiv.1607.05618	text	January 2016

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