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 ${Ba}_{2} {CuSi}_{2} O_{6} {Cl}_{2}$

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.  https://doi.org/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.  https://doi.org/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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Works referencing / citing this record:

Triplon band splitting and topologically protected edge states in the dimerized antiferromagnet
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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

Field-induced magnetic ordering in the quantum spin system KCuCl 3 journal, September 2002

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

Pressure-Induced Magnetic Quantum Phase Transition in Gapped Spin System KCuCl 3 journal, June 2006

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

Bose-Einstein Condensation in a Gas of Sodium Atoms journal, November 1995

Magnetostriction and magnetic texture to 100.75 Tesla in frustrated SrCu2(BO3)2 journal, July 2012

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

wannier90: A tool for obtaining maximally-localised Wannier functions journal, May 2008

Moriya’s anisotropic superexchange interaction, frustration, and Dzyaloshinsky’s weak ferromagnetism journal, August 1992

Bose–Einstein condensation of the triplet states in the magnetic insulator TlCuCl3 journal, May 2003

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

Magnetic Couplings in CsV 2 O 5 : A New Picture journal, April 2011

Maximally localized generalized Wannier functions for composite energy bands journal, November 1997

Pressure-Induced Quantum Phase Transition in the Spin-Liquid T l C u C l 3 journal, December 2004

Pressure-Induced Successive Magnetic Phase Transitions in the Spin Gap System TlCuCl 3 journal, June 2004

Magnetic-Field Induced Bose–Einstein Condensation of Magnons and Critical Behavior in Interacting Spin Dimer System TlCuCl 3 journal, January 2008

Plancks Gesetz und Lichtquantenhypothese journal, December 1924

Bose–Einstein condensation in magnetic insulators journal, March 2008

Quantum magnetism and criticality journal, March 2008

Long range order and metastability in two dimensional solids and superfluids. (Application of dislocation theory) journal, June 1972

QUANTUM MECHANICS: To Condense or Not to Condense journal, October 2002

Density functional approach for the magnetism of β -TeVO 4 journal, March 2014

Almost Perfect Frustration in the Dimer Magnet Ba 2 CoSi 2 O 6 Cl 2 journal, October 2014

Field- and pressure-induced magnetic quantum phase transitions in TlCuCl 3 journal, February 2004

Single-band Hubbard model with spin-orbit coupling journal, December 1983

Field-induced three-dimensional magnetic ordering in the spin-gap system journal, January 1999

Exciton–polariton condensates journal, October 2014

Bose-Einstein condensation in quantum magnets journal, May 2014

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

Pseudopotentials for high-throughput DFT calculations journal, January 2014

Linear response approach to the calculation of the effective interaction parameters in the LDA + U method journal, January 2005

Neutron Diffraction Study of the Pressure-Induced Magnetic Ordering in the Spin Gap System TlCuCl 3 journal, May 2003

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

Erratum: Direct measurement of spin correlations using magnetostriction [Phys. Rev. B. 77 , 020404(R) (2008)] journal, March 2011

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

Bose-Einstein Condensation of Dilute Magnons in TlCuCl 3 journal, June 2000

Interplay between Structural, Electronic, and Magnetic Degrees of Freedom in Sr 3 Cr 2 O 8 journal, July 2010

Anisotropic Superexchange Interaction and Weak Ferromagnetism journal, October 1960

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

Triplon band splitting and topologically protected edge states in the dimerized antiferromagnet journal, May 2019

Magnetic dimerization in the frustrated spin ladder Li 2 Cu 2 O ( SO 4 ) 2 journal, November 2017

Fiber Bragg Grating Dilatometry in Extreme Magnetic Field and Cryogenic Conditions journal, November 2017

Triplon band splitting and topologically protected edge states in the dimerized antiferromagnet text, January 2018

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

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

Field-induced magnetic ordering in the quantum spin system ${KCuCl}_{3}$
journal, September 2002

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

Pressure-Induced Magnetic Quantum Phase Transition in Gapped Spin System KCuCl ₃
journal, June 2006

Experimental Evidence for Kaplan–Shekhtman–Entin-Wohlman–Aharony Interactions in ${Ba}_{2} {CuGe}_{2} O_{7}$
journal, December 1998

Bose-Einstein Condensation in a Gas of Sodium Atoms
journal, November 1995

Magnetostriction and magnetic texture to 100.75 Tesla in frustrated SrCu2(BO3)2
journal, July 2012

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

wannier90: A tool for obtaining maximally-localised Wannier functions
journal, May 2008

Moriya’s anisotropic superexchange interaction, frustration, and Dzyaloshinsky’s weak ferromagnetism
journal, August 1992

Bose–Einstein condensation of the triplet states in the magnetic insulator TlCuCl3
journal, May 2003

Magnetic-Field-Induced Condensation of Triplons in Han Purple Pigment ${B a C u S i}_{2} O_{6}$
journal, August 2004

Magnetic Couplings in ${CsV}_{2} O_{5}$ : A New Picture
journal, April 2011

Maximally localized generalized Wannier functions for composite energy bands
journal, November 1997

Pressure-Induced Quantum Phase Transition in the Spin-Liquid $T l C u {C l}_{3}$
journal, December 2004

Pressure-Induced Successive Magnetic Phase Transitions in the Spin Gap System TlCuCl ₃
journal, June 2004

Magnetic-Field Induced Bose–Einstein Condensation of Magnons and Critical Behavior in Interacting Spin Dimer System TlCuCl ₃
journal, January 2008

Plancks Gesetz und Lichtquantenhypothese
journal, December 1924

Bose–Einstein condensation in magnetic insulators
journal, March 2008

Quantum magnetism and criticality
journal, March 2008

Long range order and metastability in two dimensional solids and superfluids. (Application of dislocation theory)
journal, June 1972

QUANTUM MECHANICS: To Condense or Not to Condense
journal, October 2002

Density functional approach for the magnetism of $β$ -TeVO $_{4}$
journal, March 2014

Almost Perfect Frustration in the Dimer Magnet Ba ₂ CoSi ₂ O ₆ Cl ₂
journal, October 2014

Field- and pressure-induced magnetic quantum phase transitions in ${TlCuCl}_{3}$
journal, February 2004

Single-band Hubbard model with spin-orbit coupling
journal, December 1983

Field-induced three-dimensional magnetic ordering in the spin-gap system
journal, January 1999

Exciton–polariton condensates
journal, October 2014

Bose-Einstein condensation in quantum magnets
journal, May 2014

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

Pseudopotentials for high-throughput DFT calculations
journal, January 2014

Linear response approach to the calculation of the effective interaction parameters in the $LDA + U$ method
journal, January 2005

Neutron Diffraction Study of the Pressure-Induced Magnetic Ordering in the Spin Gap System TlCuCl ₃
journal, May 2003

Multiple Magnon Modes and Consequences for the Bose-Einstein Condensed Phase in ${BaCuSi}_{2} O_{6}$
journal, January 2007

Erratum: Direct measurement of spin correlations using magnetostriction [Phys. Rev. B. 77 , 020404(R) (2008)]
journal, March 2011

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

Bose-Einstein Condensation of Dilute Magnons in ${TlCuCl}_{3}$
journal, June 2000

Interplay between Structural, Electronic, and Magnetic Degrees of Freedom in ${Sr}_{3} {Cr}_{2} O_{8}$
journal, July 2010

Anisotropic Superexchange Interaction and Weak Ferromagnetism
journal, October 1960

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

Triplon band splitting and topologically protected edge states in the dimerized antiferromagnet
journal, May 2019

Magnetic dimerization in the frustrated spin ladder ${Li}_{2} {Cu}_{2} O {({SO}_{4})}_{2}$
journal, November 2017

Fiber Bragg Grating Dilatometry in Extreme Magnetic Field and Cryogenic Conditions
journal, November 2017

Triplon band splitting and topologically protected edge states in the dimerized antiferromagnet
text, January 2018