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Title: Insights into the evolution from ferromagnetism to antiferromagnetism: A doping-dependent study of NaCrSi x Ge 2 - x O 6 ( 0 x 2 )

Abstract

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 TN=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 the magnetic properties of NaCrSixGe2-xO6 (x=0, 0.5, 1, 1.5, 2). Neutron diffraction and magnetization measurements show that replacing larger Ge with smaller Si simultaneously suppresses the ferromagnetic order. The lattice constants and the unit-cell volume contract, i.e., chemical pressure effect, and the Cr-Cr distance within the chain gradually decreases with increasing Si doping. High-resolution inelastic neutron-scattering studies of the spin waves of NaCrGe2O6 and NaCrSi2O6 indicate that replacing Ge with Si has profound effect on the intrachain coupling, whereas it has negligible effect on the interchain couplings. We compare our results, which indicate NaCrGe2O6 is magnetic quasi-one-dimensional (1D) and NaCrSi2O6 ismore » three-dimensional (3D), with LiCr(Si,Ge)2O6, where LiCrSi2O6 is proposed to be magnetic quasi-1D and LiCrGe2O6 is 3D, and discuss the different behaviors in magnetic dimensionality crossover in the context of how substituting Ge with Si fine-tunes the relative ratio between the intrachain and interchain couplings that defines the magnetic dimensionality in these materials.« less

Authors:
ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [1]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Neutron Scattering Division
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science & Technology Division
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) (SC-22)
OSTI Identifier:
1495957
Alternate Identifier(s):
OSTI ID: 1495235
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review B
Additional Journal Information:
Journal Volume: 99; Journal Issue: 6; 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

Citation Formats

Tian, Wei, Yan, Jiaqiang, and Kolesnikov, Alexander I. Insights into the evolution from ferromagnetism to antiferromagnetism: A doping-dependent study of NaCrSixGe2-xO6(0≤x≤2). United States: N. p., 2019. Web. doi:10.1103/PhysRevB.99.064427.
Tian, Wei, Yan, Jiaqiang, & Kolesnikov, Alexander I. Insights into the evolution from ferromagnetism to antiferromagnetism: A doping-dependent study of NaCrSixGe2-xO6(0≤x≤2). United States. doi:10.1103/PhysRevB.99.064427.
Tian, Wei, Yan, Jiaqiang, and Kolesnikov, Alexander I. Fri . "Insights into the evolution from ferromagnetism to antiferromagnetism: A doping-dependent study of NaCrSixGe2-xO6(0≤x≤2)". United States. doi:10.1103/PhysRevB.99.064427. https://www.osti.gov/servlets/purl/1495957.
@article{osti_1495957,
title = {Insights into the evolution from ferromagnetism to antiferromagnetism: A doping-dependent study of NaCrSixGe2-xO6(0≤x≤2)},
author = {Tian, Wei and Yan, Jiaqiang and Kolesnikov, Alexander I.},
abstractNote = {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 TN=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 the magnetic properties of NaCrSixGe2-xO6 (x=0, 0.5, 1, 1.5, 2). Neutron diffraction and magnetization measurements show that replacing larger Ge with smaller Si simultaneously suppresses the ferromagnetic order. The lattice constants and the unit-cell volume contract, i.e., chemical pressure effect, and the Cr-Cr distance within the chain gradually decreases with increasing Si doping. High-resolution inelastic neutron-scattering studies of the spin waves of NaCrGe2O6 and NaCrSi2O6 indicate that replacing Ge with Si has profound effect on the intrachain coupling, whereas it has negligible effect on the interchain couplings. We compare our results, which indicate NaCrGe2O6 is magnetic quasi-one-dimensional (1D) and NaCrSi2O6 is three-dimensional (3D), with LiCr(Si,Ge)2O6, where LiCrSi2O6 is proposed to be magnetic quasi-1D and LiCrGe2O6 is 3D, and discuss the different behaviors in magnetic dimensionality crossover in the context of how substituting Ge with Si fine-tunes the relative ratio between the intrachain and interchain couplings that defines the magnetic dimensionality in these materials.},
doi = {10.1103/PhysRevB.99.064427},
journal = {Physical Review B},
number = 6,
volume = 99,
place = {United States},
year = {2019},
month = {2}
}

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Works referenced in this record:

Novel Phase Transition in Spin-1/2 Linear Chain Systems: NaTiSi 2 O 6 and LiTiSi 2 O 6
journal, June 2002

  • Isobe, Masahiko; Ninomiya, Emi; N. Vasil'ev, Alexander
  • Journal of the Physical Society of Japan, Vol. 71, Issue 6
  • DOI: 10.1143/JPSJ.71.1423

Orbital dimerization in NaTiSi 2 O 6 : An orbital analogue of the spin-Peierls phase transition
journal, January 2004


Orbital and spin interplay in spin-gap formation in pyroxene A Ti Si 2 O 6 ( A = Na , Li )
journal, December 2004


Long-range antiferromagnetic order in the S = 1 chain compound LiVGe 2 O 6
journal, October 2000


Quenching of the Haldane gap in LiVSi2O6 and related compounds
journal, February 2007


Biquadratic Interactions and Spin-Peierls Transition in the Spin-1 Chain LiVGe 2 O 6
journal, November 1999


Revival of the magnetoelectric effect
journal, April 2005


Pyroxenes: a new class of multiferroics
journal, September 2007


SrMGe 2 O 6 (M = Mn, Co): a family of pyroxene compounds displaying multiferroicity
journal, January 2016

  • Ding, Lei; Colin, Claire V.; Darie, Céline
  • Journal of Materials Chemistry C, Vol. 4, Issue 19
  • DOI: 10.1039/C6TC00149A

Interplay between low dimensionality and magnetic frustration in the magnetoelectric pyroxenes LiCr X 2 O 6 ( X = Ge , Si )
journal, July 2010


Magnetic and magnetoelectric study of the pyroxene NaCrSi 2 O 6
journal, May 2010


Observation of multiferroic properties in pyroxene NaFeGe 2 O 6
journal, July 2012


A neutron diffraction study of crystal and low-temperature magnetic structures within the (Na,Li)FeGe2O6 pyroxene-type solid solution series
journal, May 2017

  • Redhammer, Günther J.; Senyshyn, Anatoliy; Lebernegg, Stefan
  • Physics and Chemistry of Minerals, Vol. 44, Issue 9
  • DOI: 10.1007/s00269-017-0892-3

Crystal and Magnetic Structures and Physical Properties of a New Pyroxene NaMnGe 2 O 6 Synthesized under High Pressure
journal, February 2013

  • Cheng, Jinguang; Tian, Wei; Zhou, Jianshi
  • Journal of the American Chemical Society, Vol. 135, Issue 7
  • DOI: 10.1021/ja312038g

Synthesis, TEM characterization and thermal behaviour of LiNiSi2O6 pyroxene
journal, March 2009

  • Tribaudino, Mario; Bromiley, Geoffrey; Ohashi, Haruo
  • Physics and Chemistry of Minerals, Vol. 36, Issue 9
  • DOI: 10.1007/s00269-009-0298-y

Magnetic and crystal structures of the one-dimensional ferromagnetic chain pyroxene NaCrGe 2 O 6
journal, July 2009


Magnetic pyroxenes LiCrGe 2 O 6 and LiCrSi 2 O 6 : Dimensionality crossover in a nonfrustrated S = 3 2 Heisenberg model
journal, December 2014


Long-range magnetic order in quasi-one-dimensional chromium-based ( S = 3 2 ) pyroxenes ( Li , Na ) Cr ( Si , Ge ) 2 O 6
journal, July 2005


Magnetic and crystal structures of the magnetoelectric pyroxene LiCrSi 2 O 6
journal, February 2009


Long-range magnetic order in quasi-one-dimensional NaCrSi2O6 and NaCrGe2O6 metal oxides
journal, November 2003

  • Vasil’ev, A. N.; Ignatchik, O. L.; Sokolov, A. N.
  • Journal of Experimental and Theoretical Physics Letters, Vol. 78, Issue 9
  • DOI: 10.1134/1.1641482

Chromium-based clinopyroxene-type germanates NaCrGe 2 O 6 and LiCrGe 2 O 6 at 298 K
journal, November 2008

  • Redhammer, Günther J.; Roth, Georg; Amthauer, Georg
  • Acta Crystallographica Section C Crystal Structure Communications, Vol. 64, Issue 12
  • DOI: 10.1107/S0108270108037633

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


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


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