Towards understanding the magnetic properties of the breathing pyrochlore compound Ba3Yb2Zn5O11through single-crystal studies
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Abstract
Abstract Ba3Yb2Zn5O11 is exceptional among breathing pyrochlore compounds for being in the nearly-decoupled limit where inter-tetrahedron interactions are weak, hosting isolated clusters or molecular magnet-like tetrahedra of magnetic ytterbium (Yb3+) ions. In this work, we present the study carried out on single-crystal samples of the breathing pyrochlore Ba3Yb2Zn5O11, using a variety of magnetometry and neutron scattering techniques along with theoretical modeling. We employ inelastic neutron scattering to investigate the magnetic dynamics as a function of applied field (with respect to both magnitude and direction) down to a temperature of 70 mK, where inelastic scattering reveals dispersionless bands of excitations as found in earlier powder sample studies, in good agreement with a single-tetrahedron model. However, diffuse neutron scattering at zero field and dc-susceptibility at finite field exhibit features suggesting the presence of excitations at low-energy that are not captured by the single tetrahedron model. Analysis of the local structure down to 2 K via pair distribution function analysis finds no evidence of structural disorder. We conclude that effects beyond the single tetrahedron model are important in describing the low-energy, low-temperature physics of Ba3Yb2Zn5O11, but their nature remains undetermined.
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OpenAlex topics: Advanced Condensed Matter Physics · Nuclear materials and radiation effects · High-pressure geophysics and materials
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References (61)
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1. Balents, L. Spin liquids in frustrated magnets. Nature 464, 199–208 (2010).10.1038/nature08917 ↗
2. Lacroix, C., Mendels, P. & Mila, F. Introduction to frustrated magnetism: materials, experiments, theory. Vol. 164 (Springer Berlin, Heidelberg, 2011).10.1007/978-3-642-10589-0 ↗
3. Gardner, J. S., Gingras, M. J. P. & Greedan, J. E. Magnetic pyrochlore oxides. Rev. Mod. Phys. 82, 53–107 (2010).10.1103/RevModPhys.82.53 ↗
4. Hallas, A. M., Gaudet, J. & Gaulin, B. D. Experimental insights into ground-state selection of quantum xy pyrochlores. Annu. Rev. Condens. Matter Phys. 9, 105–124 (2018).10.1146/annurev-conmatphys-031016-025218 ↗
5. Rau, J. G. & Gingras, M. J. Frustrated quantum rare-earth pyrochlores. Annu. Rev. Condens. Matter Phys. 10, 357–386 (2019).10.1146/annurev-conmatphys-022317-110520 ↗
6. Bramwell, S. T. & Gingras, M. J. P. Spin ice state in frustrated magnetic pyrochlore materials. Science 294, 1495–1501 (2001).10.1126/science.1064761 ↗
7. Udagawa, M. & Jaubert, L. Spin Ice (Springer Cham, Cham, 2021).10.1007/978-3-030-70860-3 ↗
8. Harris, M. J., Bramwell, S. T., McMorrow, D. F., Zeiske, T. & Godfrey, K. W. Geometrical frustration in the ferromagnetic pyrochlore Ho2Ti2O7. Phys. Rev. Lett. 79, 2554–2557 (1997).10.1103/PhysRevLett.79.2554 ↗
9. Bramwell, S. T. et al. Spin correlations in Ho2Ti2O7: a dipolar spin ice system. Phys. Rev. Lett. 87, 047205 (2001).10.1103/PhysRevLett.87.047205 ↗
10. Ramirez, A. P., Hayashi, A., Cava, R. J., Siddharthan, R. & Shastry, B. S. Zero-point entropy in ‘spin ice’. Nature 399, 333–335 (1999).10.1038/20619 ↗
11. Gingras, M. J. P. & McClarty, P. A. Quantum spin ice: a search for gapless quantum spin liquids in pyrochlore magnets. Rep. Prog. Phys. 77, 056501 (2014).10.1088/0034-4885/77/5/056501 ↗
12. Chang, L.-J. et al. Higgs transition from a magnetic coulomb liquid to a ferromagnet in Yb2Ti2O7. Nat. Commun. 3, 992 (2012).10.1038/ncomms1989 ↗
13. Stewart, J., Ehlers, G., Wills, A. S., Bramwell, S. T. & Gardner, J. S. Phase transitions, partial disorder and multi-k structures in Gd2Ti2O7. J. Phys. Condens. Matter 16, L321 (2004).10.1088/0953-8984/16/28/L01 ↗
14. Javanparast, B., Hao, Z., Enjalran, M. & Gingras, M. J. P. Fluctuation-driven selection at criticality in a frustrated magnetic system: the case of multiple-k partial order on the pyrochlore lattice. Phys. Rev. Lett. 114, 130601 (2015).10.1103/PhysRevLett.114.130601 ↗
15. Zhitomirsky, M. E., Gvozdikova, M. V., Holdsworth, P. C. W. & Moessner, R. Quantum order by disorder and accidental soft mode in Er2Ti2O7. Phys. Rev. Lett. 109, 077204 (2012).10.1103/PhysRevLett.109.077204 ↗
16. Savary, L., Ross, K. A., Gaulin, B. D., Ruff, J. P. C. & Balents, L. Order by quantum disorder in Er2Ti2O7. Phys. Rev. Lett. 109, 167201 (2012).10.1103/PhysRevLett.109.167201 ↗
17. Rau, J. G., Petit, S. & Gingras, M. J. P. Order by virtual crystal field fluctuations in pyrochlore xy antiferromagnets. Phys. Rev. B 93, 184408 (2016).10.1103/PhysRevB.93.184408 ↗
18. Oitmaa, J. et al. Phase transition and thermal order-by-disorder in the pyrochlore antiferromagnet Er2Ti2O7: a high-temperature series expansion study. Phys. Rev. B 88, 220404 (2013).10.1103/PhysRevB.88.220404 ↗
19. Gardner, J. S. et al. Cooperative paramagnetism in the geometrically frustrated pyrochlore antiferromagnet Tb2Ti2O7. Phys. Rev. Lett. 82, 1012–1015 (1999).10.1103/PhysRevLett.82.1012 ↗
20. Kimura, K. et al. Quantum fluctuations in spin-ice-like Pr2Zr2O7. Nat. Commun. 4, 1934 (2013).10.1038/ncomms2914 ↗
21. Gao, B. et al. Experimental signatures of a three-dimensional quantum spin liquid in effective spin-1/2 Ce2Zr2O7 pyrochlore. Nat. Phys. 15, 1052–1057 (2019).10.1038/s41567-019-0577-6 ↗
22. Lee, S. et al. Multistage symmetry breaking in the breathing pyrochlore lattice Li(Ga, In)Cr4O8. Phys. Rev. B 93, 174402 (2016).10.1103/PhysRevB.93.174402 ↗
23. Okamoto, Y., Nilsen, G. J., Attfield, J. P. & Hiroi, Z. Breathing pyrochlore lattice realized in a-site ordered spinel oxides LiGaCr4O8 and LiInCr4O8. Phys. Rev. Lett. 110, 097203 (2013).10.1103/PhysRevLett.110.097203 ↗
24. Okamoto, Y., Nilsen, G. J., Nakazono, T. & Hiroi, Z. Magnetic phase diagram of the breathing pyrochlore antiferromagnet LiGa1−xInxCr4O8. J. Phys. Soc. Jpn. 84, 043707 (2015).10.7566/JPSJ.84.043707 ↗
25. Okamoto, Y. et al. Magnetic and structural properties of a-site ordered chromium spinel sulfides: alternating antiferromagnetic and ferromagnetic interactions in the breathing pyrochlore lattice. J. Phys. Soc. Jpn. 87, 034709 (2018).10.7566/JPSJ.87.034709 ↗
26. Pokharel, G. et al. Negative thermal expansion and magnetoelastic coupling in the breathing pyrochlore lattice material LiGaCr4S8. Phys. Rev. B 97, 134117 (2018).10.1103/PhysRevB.97.134117 ↗
27. Pinch, H., Woods, M. & Lopatin, E. Some new mixed a-site chromium chalcogenide spinels. Mater. Res. Bull. 5, 425–429 (1970).10.1016/0025-5408(70)90081-4 ↗
28. Ghosh, P. et al. Breathing chromium spinels: a showcase for a variety of pyrochlore Heisenberg hamiltonians. npj Quantum Mater. 4, 63 (2019).10.1038/s41535-019-0202-z ↗
29. Kimura, K., Nakatsuji, S. & Kimura, T. Experimental realization of a quantum breathing pyrochlore antiferromagnet. Phys. Rev. B 90, 060414 (2014).10.1103/PhysRevB.90.060414 ↗
30. Rau, J. G. et al. Anisotropic exchange within decoupled tetrahedra in the quantum breathing pyrochlore Ba3Yb2Zn5O11. Phys. Rev. Lett. 116, 257204 (2016).10.1103/PhysRevLett.116.257204 ↗
31. Haku, T. et al. Low-energy excitations and ground-state selection in the quantum breathing pyrochlore antiferromagnet Ba3Yb2Zn5O11. Phys. Rev. B 93, 220407 (2016).10.1103/PhysRevB.93.220407 ↗
32. Haku, T. et al. Crystal field excitations in the breathing pyrochlore antiferromagnet Ba3Yb2Zn5O11. J. Phys. Soc. Jpn. 85, 034721 (2016).10.7566/JPSJ.85.034721 ↗
33. Park, S.-Y. et al. Spin–orbit coupled molecular quantum magnetism realized in inorganic solid. Nat. Commun. 7, 12912 (2016).10.1038/ncomms12912 ↗
34. Rau, J. G. & Gingras, M. J. P. Frustration and anisotropic exchange in ytterbium magnets with edge-shared octahedra. Phys. Rev. B 98, 054408 (2018).10.1103/PhysRevB.98.054408 ↗
35. Rau, J. G. et al. Behavior of the breathing pyrochlore lattice Ba3Yb2Zn5O11 in applied magnetic field. J. Phys. Condens. Matter 30, 455801 (2018).10.1088/1361-648X/aae45a ↗
36. Higo, T. et al. Frustrated magnetism in the Heisenberg pyrochlore antiferromagnets AYb2X4 (A = Cd, Mg; X = S, Se). Phys. Rev. B 95, 174443 (2017).10.1103/PhysRevB.95.174443 ↗
37. Dalmas de Réotier, P. et al. Long-range dynamical magnetic order and spin tunneling in the cooperative paramagnetic states of the pyrochlore analogous spinel antiferromagnets $${{{{{\rm{CdYb}}}}}2X}4$$(x = S or Se). Phys. Rev. B 96, 134403 (2017).10.1103/PhysRevB.96.134403 ↗
38. Guratinder, K. et al. Multiphase competition in the quantum xy pyrochlore antiferromagnet CdYb2Se4: Zero and applied magnetic field study. Phys. Rev. B 100, 094420 (2019).10.1103/PhysRevB.100.094420 ↗
39. Xing, J. et al. Néel-type antiferromagnetic order and magnetic field–temperature phase diagram in the spin $$\frac{1}{2}$$ rare-earth honeycomb compound YbCl3. Phys. Rev. B 102, 014427 (2020).10.1103/PhysRevB.102.014427 ↗
40. Sala, G. et al. Crystal field splitting, local anisotropy, and low-energy excitations in the quantum magnet YbCl3. Phys. Rev. B 100, 180406 (2019).10.1103/PhysRevB.100.180406 ↗
41. Sala, G. et al. Van Hove singularity in the magnon spectrum of the antiferromagnetic quantum honeycomb lattice. Nat. Commun. 12, 171 (2021).10.1038/s41467-020-20335-5 ↗
42. Li, F.-Y. et al. Weyl magnons in breathing pyrochlore antiferromagnets. Nat. Commun. 7, 12691 (2016).10.1038/ncomms12691 ↗
43. Savary, L. et al. Quantum spin ice on the breathing pyrochlore lattice. Phys. Rev. B 94, 075146 (2016).10.1103/PhysRevB.94.075146 ↗
44. Yan, H., Benton, O., Jaubert, L. D. C. & Shannon, N. Rank–2 U(1) spin liquid on the breathing pyrochlore lattice. Phys. Rev. Lett. 124, 127203 (2020).10.1103/PhysRevLett.124.127203 ↗
45. Haravifard, S. et al. Crystallization of spin superlattices with pressure and field in the layered magnet SrCu2(BO3)2. Nat. Commun. 7, 11956– (2016).10.1038/ncomms11956 ↗
46. Shi, Z. et al. Emergent bound states and impurity pairs in chemically doped Shastry-Sutherland system. Nat. Commun. 10, 2439 (2019).10.1038/s41467-019-10410-x ↗
47. Steinhardt, W. et al. Constraining the parameter space of a quantum spin liquid candidate in applied field with iterative optimization. Phys. Rev. Res. 3, 033050 (2021).10.1103/PhysRevResearch.3.033050 ↗
48. Landau, L. D. & Lifshitz, E. M. Quantum Mechanics, Course of Theoretical Physics, Vol.3 (Pergamon Press, Oxford, 1977).
49. Egami, T. & Billinge, S. J. Underneath the Bragg Peaks Ch.3 (Pergamon, Oxford, 2012).
50. Farrow, C. L. et al. PDFfit2 and PDFgui: computer programs for studying nanostructure in crystals. J. Phys. Condens. Matter 19, 335219 (2007).10.1088/0953-8984/19/33/335219 ↗
51. Toby, B. H. R factors in Rietveld analysis: how good is good enough? Powder Diffr. 21, 67–70 (2006).10.1154/1.2179804 ↗
52. Müller, P., Herbst-Irmer, R., Spek, A. L., Schneider, T. R. & Sawaya, M. R. Crystal Structure Refinement: a Crystallographer’s Guide to SHELXL (Oxford University Press, Oxford, 2006).10.1093/acprof:oso/9780198570769.001.0001 ↗
53. Wilson, A. J. C. (ed.) International Tables for Crystallography. Vol. C, Mathematical, physical and chemical tables (Kluwer Academic Publishers, Dordrecht/Boston/London, 1992).
54. Mirebeau, I. et al. Pressure-induced crystallization of a spin liquid. Nature 420, 54–57 (2002).10.1038/nature01157 ↗
55. Mirebeau, I., Goncharenko, I. N., Dhalenne, G. & Revcolevschi, A. Pressure and field induced magnetic order in the spin liquid Tb2Ti2O7 as studied by single crystal neutron diffraction. Phys. Rev. Lett. 93, 187204 (2004).10.1103/PhysRevLett.93.187204 ↗
56. Van Degrift, C. T. Tunnel diode oscillator for 0.001 ppm measurements at low temperatures. Rev. Sci. Instrum. 46, 599–607 (1975).10.1063/1.1134272 ↗
57. Azuah, R. T. et al. DAVE: a comprehensive software suite for the reduction, visualization, and analysis of low energy neutron spectroscopic data. J. Res. Natl Inst. Stand. Technol. 114, 341 (2009).10.6028/jres.114.025 ↗
58. Arnold, O. et al. Mantid—data analysis and visualization package for neutron scattering and μSR experiments. Nucl. Instrum. Methods Phys. Res. A 764, 156–166 (2014).10.1016/j.nima.2014.07.029 ↗
59. Molavian, H. R., Gingras, M. J. P. & Canals, B. Dynamically induced frustration as a route to a quantum spin ice state in Tb2Ti2O7 via virtual crystal field excitations and quantum many-body effects. Phys. Rev. Lett. 98, 157204 (2007).10.1103/PhysRevLett.98.157204 ↗
60. Aroyo, M. I. (ed.) International Tables for Crystallography. Vol. A, Space Group Symmetry (International Union of Crystallography, 2016), 2nd edn.10.1107/97809553602060000114 ↗
61. Ross, K. A., Savary, L., Gaulin, B. D. & Balents, L. Quantum excitations in quantum spin ice. Phys. Rev. X 1, 021002 (2011).