Quasi-two-dimensional Bose-Einstein condensation of spin triplets in the dimerized quantum magnet Ba2CuSi2O6Cl2

Okada, Makiko; Tanaka, Hidekazu; Kurita, Nobuyuki; Johmoto, Kohei; Uekusa, Hidehiro; Miyake, Atsushi; Tokunaga, Masashi; Nishimoto, Satoshi; Nakamura, Masaaki; Jaime, Marcelo; Radtke, Guillaume; Saul, Andres

doi:10.1103/PhysRevB.94.094421

Title: Quasi-two-dimensional Bose-Einstein condensation of spin triplets in the dimerized quantum magnet ${Ba}_{2} {CuSi}_{2} O_{6} {Cl}_{2}$

Journal Article · 19 September 2016 · Physical Review B

DOI: https://doi.org/10.1103/PhysRevB.94.094421 · OSTI ID:1343717

Okada, Makiko ^[1]; Tanaka, Hidekazu ^[1]; Kurita, Nobuyuki ^[1]; Johmoto, Kohei ^[1]; Uekusa, Hidehiro ^[1]; Miyake, Atsushi ^[2]; Tokunaga, Masashi ^[2]; Nishimoto, Satoshi ^[3]; Nakamura, Masaaki ^[4];

^[5]; Radtke, Guillaume ^[6]; Saul, Andres ^[7]

Tokyo Institute of Technology, Tokyo (Japan)
Univ. of Tokyo, Chiba (Japan)
IFW Dresden, Dresden (Germany); Technical Univ. Dresden, Dresden (Germany)
Ehime Univ., Ehime (Japan)
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Sorbonne Univ., Univ. Pierre et Marie Curie - Paris 6, Paris (France)
Aix-Marseille Univ., Marseille Cedex 9 (France)

We synthesized single crystals of composition Ba₂CuSi₂O₆Cl₂ and investigated their quantum magnetic properties. The crystal structure is closely related to that of the quasi-two-dimensional (2D) dimerized magnet BaCuSi₂O₆ also known as Han purple. Ba₂CuSi₂O₆Cl₂ has a singlet ground state with an excitation gap of Δ/k_B = 20.8 K. The magnetization curves for two different field directions almost perfectly coincide when normalized by the g factor except for a small jump anomaly for a magnetic field perpendicular to the c axis. The magnetization curve with a nonlinear slope above the critical field is in excellent agreement with exact-diagonalization calculations based on a 2D coupled spin-dimer model. Individual exchange constants are also evaluated using density functional theory (DFT). The DFT results demonstrate a 2D exchange network and weak frustration between interdimer exchange interactions, supported by weak spin-lattice coupling implied from our magnetostriction data. Lastly, the magnetic-field-induced spin ordering in Ba₂CuSi₂O₆Cl₂ is described as the quasi-2D Bose-Einstein condensation of triplets.

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Research Organization:: Los Alamos National Lab. (LANL), Los Alamos, NM (United States)

Sponsoring Organization:: USDOE

Grant/Contract Number:: AC52-06NA25396

OSTI ID:: 1343717

Report Number(s):: LA-UR--16-28415

Journal Information:: Physical Review B, Journal Name: Physical Review B Journal Issue: 9 Vol. 94; ISSN 2469-9950; ISSN PRBMDO

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

References (54)

Single-band Hubbard model with spin-orbit coupling Kaplan, T. A. Zeitschrift f�r Physik B Condensed Matter, Vol. 49, Issue 4 https://doi.org/10.1007/BF01301591	journal	December 1983
Plancks Gesetz und Lichtquantenhypothese Zeitschrift f�r Physik, Vol. 26, Issue 1 https://doi.org/10.1007/BF01327326	journal	December 1924
A thermodynamic theory of “weak” ferromagnetism of antiferromagnetics Dzyaloshinsky, I. Journal of Physics and Chemistry of Solids, Vol. 4, Issue 4 https://doi.org/10.1016/0022-3697(58)90076-3	journal	January 1958
Pseudopotentials for high-throughput DFT calculations Garrity, Kevin F.; Bennett, Joseph W.; Rabe, Karin M. Computational Materials Science, Vol. 81 https://doi.org/10.1016/j.commatsci.2013.08.053	journal	January 2014
wannier90: A tool for obtaining maximally-localised Wannier functions Mostofi, Arash A.; Yates, Jonathan R.; Lee, Young-Su Computer Physics Communications, Vol. 178, Issue 9 https://doi.org/10.1016/j.cpc.2007.11.016	journal	May 2008
The λ-Phenomenon of Liquid Helium and the Bose-Einstein Degeneracy London, F. Nature, Vol. 141, Issue 3571 https://doi.org/10.1038/141643a0	journal	April 1938
Bose–Einstein condensation of the triplet states in the magnetic insulator TlCuCl3 Rüegg, Ch.; Cavadini, N.; Furrer, A. Nature, Vol. 423, Issue 6935 https://doi.org/10.1038/nature01617	journal	May 2003
Dimensional reduction at a quantum critical point Sebastian, S. E.; Harrison, N.; Batista, C. D. Nature, Vol. 441, Issue 7093 https://doi.org/10.1038/nature04732	journal	June 2006
Evidence of a field-induced Berezinskii–Kosterlitz–Thouless scenario in a two-dimensional spin–dimer system Tutsch, U.; Wolf, B.; Wessel, S. Nature Communications, Vol. 5, Issue 1 https://doi.org/10.1038/ncomms6169	journal	October 2014
Exciton–polariton condensates Byrnes, Tim; Kim, Na Young; Yamamoto, Yoshihisa Nature Physics, Vol. 10, Issue 11 https://doi.org/10.1038/nphys3143	journal	October 2014
Bose–Einstein condensation in magnetic insulators Giamarchi, Thierry; Rüegg, Christian; Tchernyshyov, Oleg Nature Physics, Vol. 4, Issue 3 https://doi.org/10.1038/nphys893	journal	March 2008
Quantum magnetism and criticality Sachdev, Subir Nature Physics, Vol. 4, Issue 3 https://doi.org/10.1038/nphys894	journal	March 2008
High resolution magnetostriction measurements in pulsed magnetic fields using fiber Bragg gratings Daou, Ramzy; Weickert, Franziska; Nicklas, Michael Review of Scientific Instruments, Vol. 81, Issue 3 https://doi.org/10.1063/1.3356980	journal	March 2010
Magnetostriction and magnetic texture to 100.75 Tesla in frustrated SrCu2(BO3)2 Jaime, M.; Daou, R.; Crooker, S. A. Proceedings of the National Academy of Sciences, Vol. 109, Issue 31 https://doi.org/10.1073/pnas.1200743109	journal	July 2012
Long range order and metastability in two dimensional solids and superfluids. (Application of dislocation theory) Kosterlitz, J. M.; Thouless, D. J. Journal of Physics C: Solid State Physics, Vol. 5, Issue 11 https://doi.org/10.1088/0022-3719/5/11/002	journal	June 1972
Ordering, metastability and phase transitions in two-dimensional systems Kosterlitz, J M; Thouless, D J Journal of Physics C: Solid State Physics, Vol. 6, Issue 7, p. 1181-1203 https://doi.org/10.1088/0022-3719/6/7/010	journal	April 1973
Field-induced three-dimensional magnetic ordering in the spin-gap system Oosawa, A.; Ishii, M.; Tanaka, H. Journal of Physics: Condensed Matter, Vol. 11, Issue 1 https://doi.org/10.1088/0953-8984/11/1/021	journal	January 1999
QUANTUM ESPRESSO: a modular and open-source software project for quantum simulations of materials Giannozzi, Paolo; Baroni, Stefano; Bonini, Nicola Journal of Physics: Condensed Matter, Vol. 21, Issue 39, Article No. 395502 https://doi.org/10.1088/0953-8984/21/39/395502	journal	September 2009
Anisotropic Superexchange Interaction and Weak Ferromagnetism Moriya, Tôru Physical Review, Vol. 120, Issue 1 https://doi.org/10.1103/PhysRev.120.91	journal	October 1960
Special points for Brillouin-zone integrations Monkhorst, Hendrik J.; Pack, James D. Physical Review B, Vol. 13, Issue 12, p. 5188-5192 https://doi.org/10.1103/PhysRevB.13.5188	journal	June 1976
Temperature-dependent spin gap and singlet ground state in BaCuSi 2 O 6 Sasago, Y.; Uchinokura, K.; Zheludev, A. Physical Review B, Vol. 55, Issue 13 https://doi.org/10.1103/PhysRevB.55.8357	journal	April 1997
Maximally localized generalized Wannier functions for composite energy bands Marzari, Nicola; Vanderbilt, David Physical Review B, Vol. 56, Issue 20 https://doi.org/10.1103/PhysRevB.56.12847	journal	November 1997
Field-induced magnetic ordering in the quantum spin system KCuCl 3 Oosawa, A.; Takamasu, T.; Tatani, K. Physical Review B, Vol. 66, Issue 10 https://doi.org/10.1103/PhysRevB.66.104405	journal	September 2002
Field- and pressure-induced magnetic quantum phase transitions in TlCuCl 3 Matsumoto, Masashige; Normand, B.; Rice, T. M. Physical Review B, Vol. 69, Issue 5 https://doi.org/10.1103/PhysRevB.69.054423	journal	February 2004
Linear response approach to the calculation of the effective interaction parameters in the LDA + U method Cococcioni, Matteo; de Gironcoli, Stefano Physical Review B, Vol. 71, Issue 3 https://doi.org/10.1103/PhysRevB.71.035105	journal	January 2005
Quantum phase transitions in coupled dimer compounds Nohadani, Omid; Wessel, Stefan; Haas, Stephan Physical Review B, Vol. 72, Issue 2 https://doi.org/10.1103/PhysRevB.72.024440	journal	July 2005
Low-temperature structural phase transition and incommensurate lattice modulation in the spin-gap compound BaCuSi 2 O 6 Samulon, E. C.; Islam, Z.; Sebastian, S. E. Physical Review B, Vol. 73, Issue 10 https://doi.org/10.1103/PhysRevB.73.100407	journal	March 2006
Erratum: Direct measurement of spin correlations using magnetostriction [Phys. Rev. B. 77 , 020404(R) (2008)] Weickert, Franziska; Küchler, Robert; Zapf, Vivien Physical Review B, Vol. 83, Issue 9 https://doi.org/10.1103/PhysRevB.83.099901	journal	March 2011
Density functional approach for the magnetism of β -TeVO 4 Saúl, A.; Radtke, G. Physical Review B, Vol. 89, Issue 10 https://doi.org/10.1103/PhysRevB.89.104414	journal	March 2014
Quantum Magnets under Pressure: Controlling Elementary Excitations in TlCuCl 3 Rüegg, Ch.; Normand, B.; Matsumoto, M. Physical Review Letters, Vol. 100, Issue 20 https://doi.org/10.1103/PhysRevLett.100.205701	journal	May 2008
Interplay between Structural, Electronic, and Magnetic Degrees of Freedom in Sr 3 Cr 2 O 8 Radtke, G.; Saúl, A.; Dabkowska, H. A. Physical Review Letters, Vol. 105, Issue 3 https://doi.org/10.1103/PhysRevLett.105.036401	journal	July 2010
Magnetic Couplings in CsV 2 O 5 : A New Picture Saúl, A.; Radtke, G. Physical Review Letters, Vol. 106, Issue 17 https://doi.org/10.1103/PhysRevLett.106.177203	journal	April 2011
Nonfrustrated Interlayer Order and its Relevance to the Bose-Einstein Condensation of Magnons in BaCuSi 2 O 6 Mazurenko, Vladimir V.; Valentyuk, Maria V.; Stern, Raivo Physical Review Letters, Vol. 112, Issue 10 https://doi.org/10.1103/PhysRevLett.112.107202	journal	March 2014
Moriya’s anisotropic superexchange interaction, frustration, and Dzyaloshinsky’s weak ferromagnetism Shekhtman, L.; Entin-Wohlman, O.; Aharony, Amnon Physical Review Letters, Vol. 69, Issue 5 https://doi.org/10.1103/PhysRevLett.69.836	journal	August 1992
Bose-Einstein Condensation in a Gas of Sodium Atoms Davis, K. B.; Mewes, M. -O.; Andrews, M. R. Physical Review Letters, Vol. 75, Issue 22 https://doi.org/10.1103/PhysRevLett.75.3969	journal	November 1995
Generalized Gradient Approximation Made Simple Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868 https://doi.org/10.1103/PhysRevLett.77.3865	journal	October 1996
Experimental Evidence for Kaplan–Shekhtman–Entin-Wohlman–Aharony Interactions in Ba 2 CuGe 2 O 7 Zheludev, A.; Maslov, S.; Tsukada, I. Physical Review Letters, Vol. 81, Issue 24 https://doi.org/10.1103/PhysRevLett.81.5410	journal	December 1998
Bose-Einstein Condensation of Dilute Magnons in TlCuCl 3 Nikuni, T.; Oshikawa, M.; Oosawa, A. Physical Review Letters, Vol. 84, Issue 25 https://doi.org/10.1103/PhysRevLett.84.5868	journal	June 2000
Magnetic-Field-Induced Condensation of Triplons in Han Purple Pigment B a C u S i 2 O 6 Jaime, M.; Correa, V. F.; Harrison, N. Physical Review Letters, Vol. 93, Issue 8 https://doi.org/10.1103/PhysRevLett.93.087203	journal	August 2004
Pressure-Induced Quantum Phase Transition in the Spin-Liquid T l C u C l 3 Rüegg, Ch.; Furrer, A.; Sheptyakov, D. Physical Review Letters, Vol. 93, Issue 25 https://doi.org/10.1103/PhysRevLett.93.257201	journal	December 2004
Density Functional Theory in Transition-Metal Chemistry: A Self-Consistent Hubbard U Approach Kulik, Heather J.; Cococcioni, Matteo; Scherlis, Damian A. Physical Review Letters, Vol. 97, Issue 10 https://doi.org/10.1103/PhysRevLett.97.103001	journal	September 2006
Multiple Magnon Modes and Consequences for the Bose-Einstein Condensed Phase in BaCuSi 2 O 6 Rüegg, Ch.; McMorrow, D. F.; Normand, B. Physical Review Letters, Vol. 98, Issue 1 https://doi.org/10.1103/PhysRevLett.98.017202	journal	January 2007
Exciton-polariton Bose-Einstein condensation Deng, Hui; Haug, Hartmut; Yamamoto, Yoshihisa Reviews of Modern Physics, Vol. 82, Issue 2 https://doi.org/10.1103/RevModPhys.82.1489	journal	May 2010
Bose-Einstein condensation in quantum magnets Zapf, Vivien; Jaime, Marcelo; Batista, C. D. Reviews of Modern Physics, Vol. 86, Issue 2 https://doi.org/10.1103/RevModPhys.86.563	journal	May 2014
Reinvestigation of the structure of BaCuSi ₂ O ₆ – evidence for a phase transition at high temperature Sparta, Karine M.; Roth, Georg Acta Crystallographica Section B Structural Science, Vol. 60, Issue 5 https://doi.org/10.1107/S0108768104011644	journal	September 2004
QUANTUM MECHANICS: To Condense or Not to Condense Rice, T. M. Science, Vol. 298, Issue 5594 https://doi.org/10.1126/science.1078819	journal	October 2002
Observation of Bose-Einstein Condensation in a Dilute Atomic Vapor Anderson, M. H.; Ensher, J. R.; Matthews, M. R. Science, Vol. 269, Issue 5221 https://doi.org/10.1126/science.269.5221.198	journal	July 1995
Neutron Diffraction Study of the Pressure-Induced Magnetic Ordering in the Spin Gap System TlCuCl ₃ Oosawa, Akira; Fujisawa, Masashi; Osakabe, Toyotaka Journal of the Physical Society of Japan, Vol. 72, Issue 5 https://doi.org/10.1143/JPSJ.72.1026	journal	May 2003
Pressure-Induced Successive Magnetic Phase Transitions in the Spin Gap System TlCuCl ₃ Oosawa, Akira; Kakurai, Kazuhisa; Osakabe, Toyotaka Journal of the Physical Society of Japan, Vol. 73, Issue 6 https://doi.org/10.1143/JPSJ.73.1446	journal	June 2004
Pressure-induced Magnetic Quantum Phase Transition from Gapped Ground State in TlCuCl ₃ Goto, Kenji; Fujisawa, Masashi; Ono, Toshio Journal of the Physical Society of Japan, Vol. 73, Issue 12 https://doi.org/10.1143/JPSJ.73.3254	journal	December 2004
Pressure-Induced Magnetic Quantum Phase Transition in Gapped Spin System KCuCl ₃ Goto, Kenji; Fujisawa, Masashi; Tanaka, Hidekazu Journal of the Physical Society of Japan, Vol. 75, Issue 6 https://doi.org/10.1143/JPSJ.75.064703	journal	June 2006
Magnetic-Field Induced Bose–Einstein Condensation of Magnons and Critical Behavior in Interacting Spin Dimer System TlCuCl ₃ Yamada, Fumiko; Ono, Toshio; Tanaka, Hidekazu Journal of the Physical Society of Japan, Vol. 77, Issue 1 https://doi.org/10.1143/JPSJ.77.013701	journal	January 2008
Amplitude/Higgs Modes in Condensed Matter Physics Pekker, David; Varma, C. M. Annual Review of Condensed Matter Physics, Vol. 6, Issue 1 https://doi.org/10.1146/annurev-conmatphys-031214-014350	journal	March 2015
Almost Perfect Frustration in the Dimer Magnet Ba ₂ CoSi ₂ O ₆ Cl ₂ Tanaka, Hidekazu; Kurita, Nobuyuki; Okada, Makiko Journal of the Physical Society of Japan, Vol. 83, Issue 10 https://doi.org/10.7566/JPSJ.83.103701	journal	October 2014

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