Insights into the evolution from ferromagnetism to antiferromagnetism: A doping-dependent study of NaCrSixGe2-xO6(0≤x≤2)

Tian, Wei; Yan, Jiaqiang; Kolesnikov, Alexander I.

doi:10.1103/PhysRevB.99.064427

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

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 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 the magnetic properties of NaCrSi_xGe_2-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 »« less

Authors:

^[1];

^[2];

^[1]

Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Neutron Scattering Division
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science & Technology Division

Publication Date:: 2019-02-01

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:: 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.

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                    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.  https://doi.org/10.1103/PhysRevB.99.064427

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                    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.  https://doi.org/10.1103/PhysRevB.99.064427.  https://www.osti.gov/servlets/purl/1495957.

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@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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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

Citation Formats

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

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Orbital dimerization in ${NaTiSi}_{2} O_{6} :$ An orbital analogue of the spin-Peierls phase transition
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Orbital and spin interplay in spin-gap formation in pyroxene $A Ti {Si}_{2} O_{6}$ $(A = Na, Li)$
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Long-range antiferromagnetic order in the $S = 1$ chain compound ${LiVGe}_{2} O_{6}$
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Biquadratic Interactions and Spin-Peierls Transition in the Spin-1 Chain ${LiVGe}_{2} O_{6}$
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