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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

NaCrGe 2O 6 and NaCrSi 2O 6 are isostructural compounds exhibiting different magnetic ground states. NaCrGe2O6 adopts a ferromagnetic ground state with Tc=6K, whereas NaCrSi 2O 6 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-xO 6 (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 NaCrGe 2O 6 and NaCrSi 2O 6 indicate that replacing Ge with Si has profound effect on the intrachain coupling, whereas it has negligible effect on the interchain couplings.more » We compare our results, which indicate NaCrGe 2O 6 is magnetic quasi-one-dimensional (1D) and NaCrSi 2O 6 is three-dimensional (3D), with LiCr(Si,Ge) 2O 6, where LiCrSi 2O 6 is proposed to be magnetic quasi-1D and LiCrGe 2O 6 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.
@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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This content will become publicly available on February 1, 2020
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