skip to main content
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Magnetic ground state and magnetic excitations in black dioptase Cu 6 Si 6 O 18

Abstract

The low-temperature magnetic properties and magnetic structure of fully dehydrated black dioptase Cu 6 Si 6 O 18 have been studied by single-crystal neutron diffraction and magnetization measurements in magnetic fields up to 30 T. Here, the intrachain J c and interchain J a b interactions as well as the anisotropy of the exchange coupling J c have been determined using inelastic neutron-scattering techniques. Zero-field antiferromagnetic order at T N = 6.7 K can be described by a commensurate propagation vector of k = ( 0 , 0 , 3 / 2 ) with respect to the hexagonal R 3 ¯ :H unit cell. The Cu magnetic moments are aligned antiferromagnetically along the c axis with about 12 ° tilt and are coupled ferromagnetically between the chains. The high-field magnetization measurements provide strong evidence for the presence of a spin-flop phase above 8 T. We found that J c in black dioptase is significantly increased, while J a b is much weaker compared to its counterpart, green dioptase Cu 6 [ Si 6 O 18 ] 6 H 2 O . We suggest that black dioptase behaves like a nearly ideal S = 1 / 2 antiferromagnetic Heisenberg spiral chain with enhanced quantum fluctuations and weak spinon confinement J a b / J c ~ 0.02 .

Authors:
ORCiD logo [1];  [2];  [3]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1];  [4];  [5];  [5]; ORCiD logo [1]; ORCiD logo [1]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  2. Helmholtz-Zentrum Berlin für Materialien und Energie, Berlin (Germany)
  3. Max Planck Institute for Chemical Physics of Solids, Dresden (Germany); Technische Univ. Dresden (Germany)
  4. National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States)
  5. Tohoku Univ., Sendai (Japan)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1607105
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review B
Additional Journal Information:
Journal Volume: 100; 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; magnetic interactions; magnetism; 1-dimensional spin chains; antiferromagnets; inelastic neutron scattering; neutron scattering

Citation Formats

Podlesnyak, Andrey A., Prokhnenko, Oleksandr, Nikitin, Stanislav E., Kolesnikov, Alexander I., Matsuda, Masaaki, Dissanayake, Sachith E., Prisk, T. R., Nojiri, H., Díaz-Ortega, I. F., Kidder, Michelle K., and Anovitz, Lawrence M. Magnetic ground state and magnetic excitations in black dioptase Cu6Si6O18. United States: N. p., 2019. Web. https://doi.org/10.1103/PhysRevB.100.184401.
Podlesnyak, Andrey A., Prokhnenko, Oleksandr, Nikitin, Stanislav E., Kolesnikov, Alexander I., Matsuda, Masaaki, Dissanayake, Sachith E., Prisk, T. R., Nojiri, H., Díaz-Ortega, I. F., Kidder, Michelle K., & Anovitz, Lawrence M. Magnetic ground state and magnetic excitations in black dioptase Cu6Si6O18. United States. https://doi.org/10.1103/PhysRevB.100.184401
Podlesnyak, Andrey A., Prokhnenko, Oleksandr, Nikitin, Stanislav E., Kolesnikov, Alexander I., Matsuda, Masaaki, Dissanayake, Sachith E., Prisk, T. R., Nojiri, H., Díaz-Ortega, I. F., Kidder, Michelle K., and Anovitz, Lawrence M. Fri . "Magnetic ground state and magnetic excitations in black dioptase Cu6Si6O18". United States. https://doi.org/10.1103/PhysRevB.100.184401. https://www.osti.gov/servlets/purl/1607105.
@article{osti_1607105,
title = {Magnetic ground state and magnetic excitations in black dioptase Cu6Si6O18},
author = {Podlesnyak, Andrey A. and Prokhnenko, Oleksandr and Nikitin, Stanislav E. and Kolesnikov, Alexander I. and Matsuda, Masaaki and Dissanayake, Sachith E. and Prisk, T. R. and Nojiri, H. and Díaz-Ortega, I. F. and Kidder, Michelle K. and Anovitz, Lawrence M.},
abstractNote = {The low-temperature magnetic properties and magnetic structure of fully dehydrated black dioptase Cu6Si6O18 have been studied by single-crystal neutron diffraction and magnetization measurements in magnetic fields up to 30 T. Here, the intrachain Jc and interchain Jab interactions as well as the anisotropy of the exchange coupling Jc have been determined using inelastic neutron-scattering techniques. Zero-field antiferromagnetic order at TN=6.7 K can be described by a commensurate propagation vector of k=(0,0,3/2) with respect to the hexagonal R3¯:H unit cell. The Cu magnetic moments are aligned antiferromagnetically along the c axis with about 12° tilt and are coupled ferromagnetically between the chains. The high-field magnetization measurements provide strong evidence for the presence of a spin-flop phase above 8 T. We found that Jc in black dioptase is significantly increased, while Jab is much weaker compared to its counterpart, green dioptase Cu6[Si6O18] 6H2O. We suggest that black dioptase behaves like a nearly ideal S=1/2 antiferromagnetic Heisenberg spiral chain with enhanced quantum fluctuations and weak spinon confinement Jab/Jc~0.02.},
doi = {10.1103/PhysRevB.100.184401},
journal = {Physical Review B},
number = 18,
volume = 100,
place = {United States},
year = {2019},
month = {11}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 1 work
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

Experiments on ladders reveal a complex interplay between a spin-gapped normal state and superconductivity
journal, November 1999


The spin-1/2 Heisenberg chain: thermodynamics, quantum criticality and spin-Peierls exponents
journal, October 1998


Quantum magnetism in minerals
journal, July 2018


Spin-Wave Spectrum of the Antiferromagnetic Linear Chain
journal, December 1962


Spin liquids in frustrated magnets
journal, March 2010


Energy Separation of Single-Particle and Continuum States in an S = 1 / 2 Weakly Coupled Chains Antiferromagnet
journal, November 2000


Mantid—Data analysis and visualization package for neutron scattering and μ SR experiments
journal, November 2014

  • Arnold, O.; Bilheux, J. C.; Borreguero, J. M.
  • Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment, Vol. 764
  • DOI: 10.1016/j.nima.2014.07.029

Stochastic series expansion method with operator-loop update
journal, June 1999


Description of Anhydrous (Black) Dioptase as a S = 1/2 Uniform Antiferromagnetic Chain System
journal, January 2010

  • Law, Joseph M.; Hoch, Constantin; Whangbo, Myung-Hwan
  • Zeitschrift für anorganische und allgemeine Chemie, Vol. 636, Issue 1
  • DOI: 10.1002/zaac.200900403

Spinon confinement in a quasi-one-dimensional anisotropic Heisenberg magnet
journal, August 2017


Magnetic properties of green dioptase CuSiO3H2O and of black dioptase CuSiO3, and magnetic structure of black dioptase
journal, July 1993


Thermodynamic properties of copper silicate: dioptase: Cu6Si6O18·6H2O
journal, May 1993

  • Kiseleva, Irina A.; Ogorodova, Lyubov P.; Melchakova, Lyubov V.
  • The Journal of Chemical Thermodynamics, Vol. 25, Issue 5
  • DOI: 10.1006/jcht.1993.1057

SEQUOIA: A Newly Operating Chopper Spectrometer at the SNS
journal, November 2010


Generalized directed loop method for quantum Monte Carlo simulations
journal, March 2005


CuSiO 3 : A candidate system for purely oxygen antiferromagnet?
journal, July 2003


A comparison of four direct geometry time-of-flight spectrometers at the Spallation Neutron Source
journal, April 2014

  • Stone, M. B.; Niedziela, J. L.; Abernathy, D. L.
  • Review of Scientific Instruments, Vol. 85, Issue 4
  • DOI: 10.1063/1.4870050

Structural and chemical varieties of dioptase, Cu 6 [Si 6 O 18 ] · 6H 2 O: II. Structural properties
journal, January 1989


The ALPS project release 1.3: Open-source software for strongly correlated systems
journal, March 2007

  • Albuquerque, A. F.; Alet, F.; Corboz, P.
  • Journal of Magnetism and Magnetic Materials, Vol. 310, Issue 2
  • DOI: 10.1016/j.jmmm.2006.10.304

Observation of the spin-Peierls transition in linear Cu 2 + (spin-1/2) chains in an inorganic compound CuGeO 3
journal, June 1993


Recent advances in magnetic structure determination by neutron powder diffraction
journal, October 1993


Magnetic susceptibility measurement under high pressure and magnetization measurement of S = 1/2 dioptase lattice antiferromagnet
journal, March 2009


Representation analysis of magnetic structures
journal, January 1968

  • Bertaut, E. F.
  • Acta Crystallographica Section A: Crystal Physics, Diffraction, Theoretical and General Crystallography, Vol. 24, Issue 1
  • DOI: 10.1107/S0567739468000306

Coupled antiferromagnetic spin- 1 2 chains in green dioptase Cu 6 [ Si 6 O 18 ] · 6 H 2 O
journal, February 2016


Crystal structure of copper polysilicate, Cu[SiO3]
journal, January 1999

  • Otto, H. H.; Meibohm, M.
  • Zeitschrift für Kristallographie - Crystalline Materials, Vol. 214, Issue 9
  • DOI: 10.1524/zkri.1999.214.9.558

VESTA 3 for three-dimensional visualization of crystal, volumetric and morphology data
journal, October 2011


Quasi-one-dimensional spin chains in CuSiO3: an EPR study
journal, October 2002

  • Sichelschmidt, J.; Baenitz, M.; Geibel, C.
  • Applied Magnetic Resonance, Vol. 23, Issue 1
  • DOI: 10.1007/BF03166185

Possibility of a spin-Peierls state in CuSiO 3 from electronic structure theory
journal, January 2001


The charge-density distribution, its multipole refinement and the antiferromagnetic structure of dioptase, Cu 6 [Si 6 O 18 ]·6H 2 O
journal, July 2002

  • Belokoneva, E. L.; Gubina, Yu. K.; Forsyth, J. B.
  • Physics and Chemistry of Minerals, Vol. 29, Issue 6
  • DOI: 10.1007/s00269-002-0246-6

Bose–Einstein condensation in magnetic insulators
journal, March 2008

  • Giamarchi, Thierry; Rüegg, Christian; Tchernyshyov, Oleg
  • Nature Physics, Vol. 4, Issue 3
  • DOI: 10.1038/nphys893

Tomonaga–Luttinger liquid behavior and spinon confinement in YbAlO3
journal, February 2019


The ALPS project release 2.0: open source software for strongly correlated systems
journal, May 2011


Zur Theorie der Metalle: I. Eigenwerte und Eigenfunktionen der linearen Atomkette
journal, March 1931


Linear spin wave theory for single-Q incommensurate magnetic structures
journal, March 2015


Novel Longitudinal Mode in the Coupled Quantum Chain Compound KCuF 3
journal, July 2000


Large quantum fluctuations in the strongly coupled spin- 1 2 chains of green dioptase Cu 6 Si 6 O 18 6 H 2 O
journal, July 2010


Fractional spinon excitations in the quantum Heisenberg antiferromagnetic chain
journal, June 2013

  • Mourigal, Martin; Enderle, Mechthild; Klöpperpieper, Axel
  • Nature Physics, Vol. 9, Issue 7
  • DOI: 10.1038/nphys2652

CuSiO 3 : A quasi-one-dimensional S = 1 2 antiferromagnetic chain system
journal, November 2000


Structural and chemical varieties of dioptase, Cu6[Si6O18] · 6 H2O I. Thermal properties
journal, January 1988

  • Breuer, K. -H.; Eysel, W.
  • Zeitschrift für Kristallographie - Crystalline Materials, Vol. 184, Issue 1-4
  • DOI: 10.1524/zkri.1988.184.14.1

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

The cold neutron chopper spectrometer at the Spallation Neutron Source—A review of the first 8 years of operation
journal, September 2016

  • Ehlers, G.; Podlesnyak, A. A.; Kolesnikov, A. I.
  • Review of Scientific Instruments, Vol. 87, Issue 9
  • DOI: 10.1063/1.4962024

Crystalline Electric-Field Randomness in the Triangular Lattice Spin-Liquid YbMgGaO 4
journal, March 2017


Horace : Software for the analysis of data from single crystal spectroscopy experiments at time-of-flight neutron instruments
journal, October 2016

  • Ewings, R. A.; Buts, A.; Le, M. D.
  • Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment, Vol. 834
  • DOI: 10.1016/j.nima.2016.07.036