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

doi:10.1103/PhysRevB.94.094421

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

Abstract

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.

Authors:

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)

Publication Date:: 2016-09-20

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

Sponsoring Org.:: USDOE

OSTI Identifier:: 1343717

Alternate Identifier(s):: OSTI ID: 1325607

Report Number(s):: LA-UR-16-28415
Journal ID: ISSN 2469-9950; PRBMDO; TRN: US1701625

Grant/Contract Number:: AC52-06NA25396

Resource Type:: Accepted Manuscript

Journal Name:: Physical Review B

Additional Journal Information:: Journal Volume: 94; Journal Issue: 9; 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; High Magnetic Field Science

Citation Formats


                    Okada, Makiko, Tanaka, Hidekazu, Kurita, Nobuyuki, Johmoto, Kohei, Uekusa, Hidehiro, Miyake, Atsushi, Tokunaga, Masashi, Nishimoto, Satoshi, Nakamura, Masaaki, Jaime, Marcelo, Radtke, Guillaume, and Saul, Andres. Quasi-two-dimensional Bose-Einstein condensation of spin triplets in the dimerized quantum magnet Ba2CuSi2O6Cl2.  United States: N. p., 2016. 
        Web.  doi:10.1103/PhysRevB.94.094421.

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                    Okada, Makiko, Tanaka, Hidekazu, Kurita, Nobuyuki, Johmoto, Kohei, Uekusa, Hidehiro, Miyake, Atsushi, Tokunaga, Masashi, Nishimoto, Satoshi, Nakamura, Masaaki, Jaime, Marcelo, Radtke, Guillaume, & Saul, Andres. Quasi-two-dimensional Bose-Einstein condensation of spin triplets in the dimerized quantum magnet Ba2CuSi2O6Cl2.  United States.  doi:10.1103/PhysRevB.94.094421.

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                    Okada, Makiko, Tanaka, Hidekazu, Kurita, Nobuyuki, Johmoto, Kohei, Uekusa, Hidehiro, Miyake, Atsushi, Tokunaga, Masashi, Nishimoto, Satoshi, Nakamura, Masaaki, Jaime, Marcelo, Radtke, Guillaume, and Saul, Andres. Tue .  
        "Quasi-two-dimensional Bose-Einstein condensation of spin triplets in the dimerized quantum magnet Ba2CuSi2O6Cl2".  United States.  doi:10.1103/PhysRevB.94.094421.  https://www.osti.gov/servlets/purl/1343717.

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@article{osti_1343717,

  title        = {Quasi-two-dimensional Bose-Einstein condensation of spin triplets in the dimerized quantum magnet Ba2CuSi2O6Cl2},

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

  abstractNote = {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/kB = 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.},

  doi          = {10.1103/PhysRevB.94.094421},

  journal      = {Physical Review B},

  number       = 9,

  volume       = 94,

  place        = {United States},

  year         = {2016},

  month        = {9}

}

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DOI: 10.1103/PhysRevB.94.094421

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Title: Quasi-two-dimensional Bose-Einstein condensation of spin triplets in the dimerized quantum magnet Ba 2 CuSi 2 O 6 Cl 2

Abstract

Citation Formats

Observation of Bose-Einstein Condensation in a Dilute Atomic Vapor journal, July 1995

Generalized Gradient Approximation Made Simple journal, October 1996

The λ-Phenomenon of Liquid Helium and the Bose-Einstein Degeneracy journal, April 1938

Dimensional reduction at a quantum critical point journal, June 2006

Exciton-polariton Bose-Einstein condensation journal, May 2010

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A thermodynamic theory of “weak” ferromagnetism of antiferromagnetics journal, January 1958

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Experimental Evidence for Kaplan–Shekhtman–Entin-Wohlman–Aharony Interactions in Ba 2 CuGe 2 O 7 journal, December 1998

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QUANTUM ESPRESSO: a modular and open-source software project for quantum simulations of materials journal, September 2009

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Magnetic-Field-Induced Condensation of Triplons in Han Purple Pigment B a C u S i 2 O 6 journal, August 2004

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Exciton–polariton condensates journal, October 2014

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Amplitude/Higgs Modes in Condensed Matter Physics journal, March 2015

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Multiple Magnon Modes and Consequences for the Bose-Einstein Condensed Phase in BaCuSi 2 O 6 journal, January 2007

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High resolution magnetostriction measurements in pulsed magnetic fields using fiber Bragg gratings journal, March 2010

Quantum phase transitions in coupled dimer compounds journal, July 2005

Pressure-induced Magnetic Quantum Phase Transition from Gapped Ground State in TlCuCl 3 journal, December 2004

Low-temperature structural phase transition and incommensurate lattice modulation in the spin-gap compound BaCuSi 2 O 6 journal, March 2006

Temperature-dependent spin gap and singlet ground state in BaCuSi 2 O 6 journal, April 1997

Special points for Brillouin-zone integrations journal, June 1976

Quantum Magnets under Pressure: Controlling Elementary Excitations in TlCuCl 3 journal, May 2008

Evidence of a field-induced Berezinskii–Kosterlitz–Thouless scenario in a two-dimensional spin–dimer system journal, October 2014

Reinvestigation of the structure of BaCuSi 2 O 6 – evidence for a phase transition at high temperature journal, September 2004

Ordering, metastability and phase transitions in two-dimensional systems journal, April 1973

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Density Functional Theory in Transition-Metal Chemistry: A Self-Consistent Hubbard U Approach journal, September 2006

Nonfrustrated Interlayer Order and its Relevance to the Bose-Einstein Condensation of Magnons in BaCuSi 2 O 6 journal, March 2014

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

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Neutron Diffraction Study of the Pressure-Induced Magnetic Ordering in the Spin Gap System TlCuCl ₃
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Multiple Magnon Modes and Consequences for the Bose-Einstein Condensed Phase in ${BaCuSi}_{2} O_{6}$
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Erratum: Direct measurement of spin correlations using magnetostriction [Phys. Rev. B. 77 , 020404(R) (2008)]
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High resolution magnetostriction measurements in pulsed magnetic fields using fiber Bragg gratings
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Quantum phase transitions in coupled dimer compounds
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Pressure-induced Magnetic Quantum Phase Transition from Gapped Ground State in TlCuCl ₃
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Low-temperature structural phase transition and incommensurate lattice modulation in the spin-gap compound ${BaCuSi}_{2} O_{6}$
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Temperature-dependent spin gap and singlet ground state in ${BaCuSi}_{2}$ $O_{6}$
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Special points for Brillouin-zone integrations
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Quantum Magnets under Pressure: Controlling Elementary Excitations in ${TlCuCl}_{3}$
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Evidence of a field-induced Berezinskii–Kosterlitz–Thouless scenario in a two-dimensional spin–dimer system
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Reinvestigation of the structure of BaCuSi ₂ O ₆ – evidence for a phase transition at high temperature
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Ordering, metastability and phase transitions in two-dimensional systems
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Bose-Einstein Condensation of Dilute Magnons in ${TlCuCl}_{3}$
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Interplay between Structural, Electronic, and Magnetic Degrees of Freedom in ${Sr}_{3} {Cr}_{2} O_{8}$
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Anisotropic Superexchange Interaction and Weak Ferromagnetism
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Density Functional Theory in Transition-Metal Chemistry: A Self-Consistent Hubbard $U$ Approach
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Nonfrustrated Interlayer Order and its Relevance to the Bose-Einstein Condensation of Magnons in ${BaCuSi}_{2} O_{6}$
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