Spin triplet ground-state in the copper hexamer compounds A2Cu3O(SO4)3(A=Na,K)

Furrer, A.; Podlesnyak, A.; Pomjakushina, E.; Pomjakushin, V.

doi:10.1103/PhysRevB.98.180410

Title: Spin triplet ground-state in the copper hexamer compounds $A_{2} C u_{3} O {(S O_{4})}_{3} (A = Na, K)$

Abstract

The compounds $${A}_{2}\mathrm{C}{\mathrm{u}}_{3}\mathrm{O}{(\mathrm{S}{\mathrm{O}}_{4})}_{3}(A=\mathrm{Na},\mathrm{K})$$ are characterized by copper hexamers which are weakly coupled along the $$b$$ axis to realize one-dimensional antiferromagnetic chains below $${T}_{\mathrm{N}}{\approx}3\mathrm{K}$$, whereas the interchain interactions along the $$a$$ and $$c$$ axes are negligible. Here we investigated the energy-level splittings of the copper hexamers by inelastic neutron scattering below and above $${T}_{\mathrm{N}}$$. The eight lowest-lying hexamer states could be unambiguously assigned and parametrized in terms of a Heisenberg exchange Hamiltonian, providing direct experimental evidence for an $S=1$ triplet ground-state associated with the copper hexamers. Therefore, the compounds $${A}_{2}\mathrm{C}{\mathrm{u}}_{3}\mathrm{O}{(\mathrm{S}{\mathrm{O}}_{4})}_{3}$$ serve as cluster-based spin-1 antiferromagnets to support Haldane's conjecture that a gap appears in the excitation spectrum below $${T}_{\mathrm{N}}$$, which was verified by inelastic neutron scattering.

Authors:

Furrer, A. ^[1]; Podlesnyak, A. ^[2]; Pomjakushina, E. ^[3]; Pomjakushin, V. ^[1]

Paul Scherrer Inst. (PSI), Villigen (Switzerland). Lab. for Neutron Scattering and Imaging
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Neutron Scattering Division
Paul Scherrer Inst. (PSI), Villigen (Switzerland). Lab. for Multiscale Materials Experiments

Publication Date:: Thu Nov 29 00:00:00 EST 2018

Research Org.:: Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Paul Scherrer Inst. (PSI), Villigen (Switzerland)

Sponsoring Org.:: USDOE Office of Science (SC)

OSTI Identifier:: 1484096

Alternate Identifier(s):: OSTI ID: 1483918

Grant/Contract Number:: AC05-00OR22725

Resource Type:: Accepted Manuscript

Journal Name:: Physical Review B

Additional Journal Information:: Journal Volume: 98; Journal Issue: 18; 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; magnetism

Citation Formats


                    Furrer, A., Podlesnyak, A., Pomjakushina, E., and Pomjakushin, V. Spin triplet ground-state in the copper hexamer compounds A2Cu3O(SO4)3(A=Na,K).  United States: N. p., 2018. 
Web.  doi:10.1103/PhysRevB.98.180410.

Copy to clipboard


                    Furrer, A., Podlesnyak, A., Pomjakushina, E., & Pomjakushin, V. Spin triplet ground-state in the copper hexamer compounds A2Cu3O(SO4)3(A=Na,K).  United States.  https://doi.org/10.1103/PhysRevB.98.180410

Copy to clipboard


                    Furrer, A., Podlesnyak, A., Pomjakushina, E., and Pomjakushin, V. Thu .  
"Spin triplet ground-state in the copper hexamer compounds A2Cu3O(SO4)3(A=Na,K)".  United States.  https://doi.org/10.1103/PhysRevB.98.180410.  https://www.osti.gov/servlets/purl/1484096.

Copy to clipboard


                    
@article{osti_1484096,

  title        = {Spin triplet ground-state in the copper hexamer compounds A2Cu3O(SO4)3(A=Na,K)},

  author       = {Furrer, A. and Podlesnyak, A. and Pomjakushina, E. and Pomjakushin, V.},

  abstractNote = {The compounds ${A}_{2}\mathrm{C}{\mathrm{u}}_{3}\mathrm{O}{(\mathrm{S}{\mathrm{O}}_{4})}_{3}(A=\mathrm{Na},\mathrm{K})$ are characterized by copper hexamers which are weakly coupled along the $b$ axis to realize one-dimensional antiferromagnetic chains below ${T}_{\mathrm{N}}{\approx}3\mathrm{K}$, whereas the interchain interactions along the $a$ and $c$ axes are negligible. Here we investigated the energy-level splittings of the copper hexamers by inelastic neutron scattering below and above ${T}_{\mathrm{N}}$. The eight lowest-lying hexamer states could be unambiguously assigned and parametrized in terms of a Heisenberg exchange Hamiltonian, providing direct experimental evidence for an $S=1$ triplet ground-state associated with the copper hexamers. Therefore, the compounds ${A}_{2}\mathrm{C}{\mathrm{u}}_{3}\mathrm{O}{(\mathrm{S}{\mathrm{O}}_{4})}_{3}$ serve as cluster-based spin-1 antiferromagnets to support Haldane's conjecture that a gap appears in the excitation spectrum below ${T}_{\mathrm{N}}$, which was verified by inelastic neutron scattering.},

  doi          = {10.1103/PhysRevB.98.180410},

  journal      = {Physical Review B},

  number       = 18,

  volume       = 98,

  place        = {United States},

  year         = {Thu Nov 29 00:00:00 EST 2018},

  month        = {Thu Nov 29 00:00:00 EST 2018}

}

Copy to clipboard

Journal Article:

Free Publicly Available Full Text

Accepted Manuscript (Publisher)

Accepted Manuscript (DOE)

Publisher's Version of Record

https://doi.org/10.1103/PhysRevB.98.180410

Other availability

Search WorldCat to find libraries that may hold this journal

Citation Metrics:

Cited by: 11 works

Citation information provided by
Web of Science

Save / Share:

Export Metadata

Save to My Library

Works referenced in this record:

Nonlinear Field Theory of Large-Spin Heisenberg Antiferromagnets: Semiclassically Quantized Solitons of the One-Dimensional Easy-Axis Néel State
journal, April 1983

Haldane, F. D. M.
Physical Review Letters, Vol. 50, Issue 15
DOI: 10.1103/PhysRevLett.50.1153

Copper oxosulphates from fumaroles of Tolbachik volcano: puninite, Na2 Cu3 O(SO4)3 –a new mineral species and structure refinements of kamchatkite and alumoklyuchevskite [Copper oxosulphates from fumaroles of Tolbachik volcano: puninite, Na2 Cu3 O(SO4)3 –a new mineral species and structure refinements of kamchatkite and alumoklyuchevskite]
journal, July 2017

Siidra, Oleg I.; Nazarchuk, Evgenii V.; Zaitsev, Anatoly N.
European Journal of Mineralogy, Vol. 29, Issue 3
DOI: 10.1127/ejm/2017/0029-2619

Colloquium : Herbertsmithite and the search for the quantum spin liquid
journal, December 2016

Norman, M. R.
Reviews of Modern Physics, Vol. 88, Issue 4
DOI: 10.1103/RevModPhys.88.041002

Antiferromagnetic ordering in Cu ₂ OCl ₂ studied by the muon spin rotation/relaxation technique
journal, March 2007

Kawashima, K.; Okabe, H.; Suzuki, K.
Journal of Physics: Condensed Matter, Vol. 19, Issue 14
DOI: 10.1088/0953-8984/19/14/145275

Magnetic structure of the $spin - \frac{1}{2}$ frustrated quasi-one-dimensional antiferromagnet ${Cu}_{3} {Mo}_{2} O_{9}$ : Appearance of a partially disordered state
journal, August 2015

Hase, Masashi; Kuroe, Haruhiko; Pomjakushin, Vladimir Yu.
Physical Review B, Vol. 92, Issue 5
DOI: 10.1103/PhysRevB.92.054425

${AgCuVO}_{4}$ : A quasi-one-dimensional $S = \frac{1}{2}$ chain compound
journal, September 2009

Möller, A.; Schmitt, M.; Schnelle, W.
Physical Review B, Vol. 80, Issue 12
DOI: 10.1103/PhysRevB.80.125106

The crystal structure of alumoklyuchevskite, K3Cu3AlO2(SO4)4
journal, December 2009

Krivovichev, S. V.; Filatov, S. K.; Cherepansky, P. N.
Geology of Ore Deposits, Vol. 51, Issue 7
DOI: 10.1134/S1075701509070149

Spin-frustrated pyrochlore chains in the volcanic mineral kamchatkite (KCu3OCl(SO4)2)
journal, February 2018

Volkova, L. M.; Marinin, D. V.
Physics and Chemistry of Minerals, Vol. 45, Issue 7
DOI: 10.1007/s00269-018-0950-5

Cluster-Based Haldane State in an Edge-Shared Tetrahedral Spin-Cluster Chain: Fedotovite $K_{2} {Cu}_{3} O ({SO}_{4})_{3}$
journal, February 2018

Fujihala, M.; Sugimoto, T.; Tohyama, T.
Physical Review Letters, Vol. 120, Issue 7
DOI: 10.1103/PhysRevLett.120.077201

Magnetic properties of a Heisenberg coupled-trimer molecular magnet: General results and application to spin- $\frac{1}{2}$ vanadium clusters
journal, August 2009

Haraldsen, J. T.; Barnes, T.; Sinclair, J. W.
Physical Review B, Vol. 80, Issue 6
DOI: 10.1103/PhysRevB.80.064406

Frustrated Cuprate Route from Antiferromagnetic to Ferromagnetic Spin- $\frac{1}{2}$ Heisenberg Chains: ${Li}_{2} {ZrCuO}_{4}$ as a Missing Link near the Quantum Critical Point
journal, February 2007

Drechsler, S. -L.; Volkova, O.; Vasiliev, A. N.
Physical Review Letters, Vol. 98, Issue 7
DOI: 10.1103/PhysRevLett.98.077202

The crystal structure of fedotovite, K ₂ Cu ₃ O(SO ₄ ) ₃
journal, December 1991

Starova, G. L.; Filatov, S. K.; Fundamensky, V. S.
Mineralogical Magazine, Vol. 55, Issue 381
DOI: 10.1180/minmag.1991.055.381.14

The new cold neutron chopper spectrometer at the Spallation Neutron Source: Design and performance
journal, August 2011

Ehlers, G.; Podlesnyak, A. A.; Niedziela, J. L.
Review of Scientific Instruments, Vol. 82, Issue 8
DOI: 10.1063/1.3626935

Antiferromagnetism. Theory of Superexchange Interaction
journal, July 1950

Anderson, P. W.
Physical Review, Vol. 79, Issue 2
DOI: 10.1103/PhysRev.79.350

Theory of the Role of Covalence in the Perovskite-Type Manganites $[La, M (II)] Mn O_{3}$
journal, October 1955

Goodenough, John B.
Physical Review, Vol. 100, Issue 2
DOI: 10.1103/PhysRev.100.564

Works referencing / citing this record:

Quantum magnetism in minerals
journal, July 2018

Inosov, D. S.
Advances in Physics, Vol. 67, Issue 3
DOI: 10.1080/00018732.2018.1571986

Cluster-based Haldane phases, bound magnon crystals and quantum spin liquids of a mixed spin-1 and spin-1/2 Heisenberg octahedral chain
journal, September 2019

Karl'ová, Katarína; Strečka, Jozef; Verkholyak, Taras
Physical Review B, Vol. 100, Issue 9
DOI: 10.1103/physrevb.100.094405

Quantum Magnetism in Minerals
text, January 2018

Inosov, D. S.
arXiv
DOI: 10.48550/arxiv.1806.10967

Cluster-based Haldane phases, bound magnon crystals and quantum spin liquids of a mixed spin-1 and spin-1/2 Heisenberg octahedral chain
text, January 2019

Karlova, Katarina; Strecka, Jozef; Verkholyak, Taras
arXiv
DOI: 10.48550/arxiv.1904.02889

Similar Records in DOE PAGES and OSTI.GOV collections:

Effect of Sr doping on the magnetic exchange interactions in manganites of type $L a_{1 - x} S r_{x} M n_{y} A_{1 - y} O_{3} (A = Ga, Ti; 0.1 \leq y \leq 1)$

Journal Article Furrer, Albert ; Podlesnyak, Andrey A. ; Pomjakushina, Ekaterina ; ... - Physical Review B

Strontium doping transforms manganites of type La _{1 - x} Sr _x Mn O ₃ from an insulating antiferromagnet ( x = 0 ) to a metallic ferromagnet ( x > 0.16 ) due to the induced charge carriers (holes). We employed neutron scattering experiments in order to investigate the effect of Sr doping on a tailor-made compound of composition La _0.7 S r _0.3 M n _0.1 Ti _0.3 G a _0.6 O ₃ . By the simultaneous doping with S r ^{2 +} and Ti^{4 +} ions, the compound remains in the insulating state so that themore »« less
Cited by 4
https://doi.org/10.1103/PhysRevB.95.104414

Full Text Available
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 Maharaj, D. D. ; Sala, G. ; Marjerrison, C. A. ; ... - Physical Review B

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 inmore »« less
Cited by 7
https://doi.org/10.1103/PhysRevB.98.104434

Full Text Available
Insights into the evolution from ferromagnetism to antiferromagnetism: A doping-dependent study of ${NaCrSi}_{x} {Ge}_{2 - x} O_{6} (0 \leq x \leq 2)$

Journal Article Tian, Wei ; Yan, Jiaqiang ; Kolesnikov, Alexander I. - Physical Review B

NaCrGe₂O₆ and NaCrSi₂O₆ are isostructural compounds exhibiting different magnetic ground states. NaCrGe2O6 adopts a ferromagnetic ground state with Tc=6K, whereas NaCrSi₂O₆ orders antiferromagnetically below T_N=3.4K. Although it has been proposed that the intriguing magnetic behavior in Cr-based pyroxenes involves competition between antiferromagnetic direct exchange and ferromagnetic superexchange interactions, a delicate balance that is sensitive to Cr-Cr distance and local distortion, no spectroscopy study has been done to determine the microscopic interactions in these compounds. To delve deeper into the evolution from ferromagnetism to antiferromagnetism, we performed a doping-dependent study to investigate how the substitution of Ge by Si affects themore »« less
https://doi.org/10.1103/PhysRevB.99.064427

Full Text Available
Evolution of magnetism in single-crystal $C a_{2} R u_{1 - x} I r_{x} O_{4} (0 \leq x \leq 0.65)$

Journal Article Yuan, S. J. ; Terzic, J. ; Wang, J. C. ; ... - Physical Review. B, Condensed Matter and Materials Physics

In this paper, we report structural, magnetic, transport, and thermal properties of single-crystal Ca₂Ru_1-xIr_xO₄(0≤x≤0.65). Ca₂RuO₄ is a structurally driven Mott insulator with a metal-insulator transition at T_MI=357K, which is well separated from antiferromagnetic order at T_N=110K. Substitution of a 5d element, Ir, for Ru enhances spin-orbit coupling and locking between the structural distortions and magnetic moment canting. Ir doping intensifies the distortion or rotation of Ru/IrO₆ octahedra and induces weak ferromagnetic behavior along the c axis. In particular, Ir doping suppresses T_N but concurrently causes an additional magnetic ordering T_N2 at a higher temperature up to 210 K for x=0.65.more »« less
Cited by 6
https://doi.org/10.1103/PhysRevB.92.024425

Full Text Available
Frustrated spin- $\frac{1}{2}$ molecular magnetism in the mixed-valence antiferromagnets ${Ba}_{3} M {Ru}_{2} O_{9} (M = In$ , Y, Lu)

Journal Article Ziat, D. ; Aczel, Adam A. ; Sinclair, R. ; ... - Physical Review B

We have performed magnetic susceptibility, heat capacity, muon spin relaxation, and neutron-scattering measurements on three members of the family Ba₃MRu₂O₉, where M=In, Y, and Lu. These systems consist of mixed-valence Ru dimers on a triangular lattice with antiferromagnetic interdimer exchange. Although previous work has argued that charge order within the dimers or intradimer double exchange plays an important role in determining the magnetic properties, our results suggest that the dimers are better described as molecular units due to significant orbital hybridization, resulting in one spin-1/2 moment distributed equally over the two Ru sites. These molecular building blocks form a frustrated,more »« less
Cited by 24
https://doi.org/10.1103/PhysRevB.95.184424

Full Text Available

Similar Records

Title: Spin triplet ground-state in the copper hexamer compounds A 2 C u 3 O ( S O 4 ) 3 ( A = Na , K )

Abstract

Citation Formats

Nonlinear Field Theory of Large-Spin Heisenberg Antiferromagnets: Semiclassically Quantized Solitons of the One-Dimensional Easy-Axis Néel State journal, April 1983

Colloquium : Herbertsmithite and the search for the quantum spin liquid journal, December 2016

Antiferromagnetic ordering in Cu 2 OCl 2 studied by the muon spin rotation/relaxation technique journal, March 2007

Magnetic structure of the spin − 1 2 frustrated quasi-one-dimensional antiferromagnet Cu 3 Mo 2 O 9 : Appearance of a partially disordered state journal, August 2015

AgCuVO 4 : A quasi-one-dimensional S = 1 2 chain compound journal, September 2009

The crystal structure of alumoklyuchevskite, K3Cu3AlO2(SO4)4 journal, December 2009

Spin-frustrated pyrochlore chains in the volcanic mineral kamchatkite (KCu3OCl(SO4)2) journal, February 2018

Cluster-Based Haldane State in an Edge-Shared Tetrahedral Spin-Cluster Chain: Fedotovite K 2 Cu 3 O ( SO 4 ) 3 journal, February 2018

Magnetic properties of a Heisenberg coupled-trimer molecular magnet: General results and application to spin- 1 2 vanadium clusters journal, August 2009

Frustrated Cuprate Route from Antiferromagnetic to Ferromagnetic Spin- 1 2 Heisenberg Chains: Li 2 ZrCuO 4 as a Missing Link near the Quantum Critical Point journal, February 2007

The crystal structure of fedotovite, K 2 Cu 3 O(SO 4 ) 3 journal, December 1991

The new cold neutron chopper spectrometer at the Spallation Neutron Source: Design and performance journal, August 2011

Antiferromagnetism. Theory of Superexchange Interaction journal, July 1950

Theory of the Role of Covalence in the Perovskite-Type Manganites [ La , M ( II ) ] Mn O 3 journal, October 1955

Quantum magnetism in minerals journal, July 2018

Cluster-based Haldane phases, bound magnon crystals and quantum spin liquids of a mixed spin-1 and spin-1/2 Heisenberg octahedral chain journal, September 2019

Quantum Magnetism in Minerals text, January 2018

Cluster-based Haldane phases, bound magnon crystals and quantum spin liquids of a mixed spin-1 and spin-1/2 Heisenberg octahedral chain text, January 2019

Title: Spin triplet ground-state in the copper hexamer compounds $A_{2} C u_{3} O {(S O_{4})}_{3} (A = Na, K)$

Nonlinear Field Theory of Large-Spin Heisenberg Antiferromagnets: Semiclassically Quantized Solitons of the One-Dimensional Easy-Axis Néel State
journal, April 1983

Colloquium : Herbertsmithite and the search for the quantum spin liquid
journal, December 2016

Antiferromagnetic ordering in Cu ₂ OCl ₂ studied by the muon spin rotation/relaxation technique
journal, March 2007

Magnetic structure of the $spin - \frac{1}{2}$ frustrated quasi-one-dimensional antiferromagnet ${Cu}_{3} {Mo}_{2} O_{9}$ : Appearance of a partially disordered state
journal, August 2015

${AgCuVO}_{4}$ : A quasi-one-dimensional $S = \frac{1}{2}$ chain compound
journal, September 2009

The crystal structure of alumoklyuchevskite, K3Cu3AlO2(SO4)4
journal, December 2009

Spin-frustrated pyrochlore chains in the volcanic mineral kamchatkite (KCu3OCl(SO4)2)
journal, February 2018

Cluster-Based Haldane State in an Edge-Shared Tetrahedral Spin-Cluster Chain: Fedotovite $K_{2} {Cu}_{3} O ({SO}_{4})_{3}$
journal, February 2018

Magnetic properties of a Heisenberg coupled-trimer molecular magnet: General results and application to spin- $\frac{1}{2}$ vanadium clusters
journal, August 2009

Frustrated Cuprate Route from Antiferromagnetic to Ferromagnetic Spin- $\frac{1}{2}$ Heisenberg Chains: ${Li}_{2} {ZrCuO}_{4}$ as a Missing Link near the Quantum Critical Point
journal, February 2007

The crystal structure of fedotovite, K ₂ Cu ₃ O(SO ₄ ) ₃
journal, December 1991

The new cold neutron chopper spectrometer at the Spallation Neutron Source: Design and performance
journal, August 2011

Antiferromagnetism. Theory of Superexchange Interaction
journal, July 1950

Theory of the Role of Covalence in the Perovskite-Type Manganites $[La, M (II)] Mn O_{3}$
journal, October 1955

Quantum magnetism in minerals
journal, July 2018

Cluster-based Haldane phases, bound magnon crystals and quantum spin liquids of a mixed spin-1 and spin-1/2 Heisenberg octahedral chain
journal, September 2019

Quantum Magnetism in Minerals
text, January 2018

Cluster-based Haldane phases, bound magnon crystals and quantum spin liquids of a mixed spin-1 and spin-1/2 Heisenberg octahedral chain
text, January 2019