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Title: Spin state and spectroscopic modes of multiferroic BiFeO 3

Abstract

Spectroscopic modes provide the most sensitive probe of the very weak interactions responsible for the properties of the long-wavelength cycloid in the multiferroic phase of BiFeO3 below TN ≈ 640 K. Three of the four modes measured by terahertz (THz) and Raman spectroscopies were recently identified using a simple microscopic model. While a Dzyaloshinskii-Moriya (DM) interaction D along [-1, 2, -1] induces a cycloid with wave vector (2π/α) (0.5 + δ, 0.5, 0.5 - δ) (δ ≈ 0.0045), easy-axis anisotropy K along the [1, 1, 1] direction of the electric polarization P induces higher harmonics of the cycloid, which split the $${\Psi}_{1}$$ modes at 2.49 and 2.67 meV and activate the $${{\Phi}}_{2}$$ mode at 3.38 meV. However, that model could not explain the observed low-frequency mode at about 2.17 meV. We now demonstrate that an additional DM interaction D' along [1, 1, 1] not only produces the observed weak ferromagnetic moment of the high-field phase above 18 T but also activates the spectroscopic matrix elements of the nearly degenerate, low-frequency $${\Psi}_{0}$$ and $${\Phi}_{1}$$ modes, although their scattering intensities remain extremely weak. Even in the absence of easy-axis anisotropy, D' produces cycloidal harmonics that split $${\Psi}_{1}$$ and activate $${\Phi}_{2}$$. However, themore » observed mode frequencies and selection rules require that both D' and K are nonzero. This work also resolves an earlier disagreement between spectroscopic and inelastic neutron-scattering measurements.« less

Authors:
 [1];  [2];  [3];  [4]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science & Technology Division
  2. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
  3. Aoyama Gakuin Univ., Sagamihara, Kanagawa (Japan). Dept. of Physics and Mathematics
  4. Pohang Univ. of Science and Technology (POSTECH), Pohang, Gyeongbuk (Korea, Republic of). Asia Pacific Center for Theoretical Physics
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). Materials Sciences & Engineering Division; USDOE National Nuclear Security Administration (NNSA); Ministry of Education, Culture, and Technology, Japan (MEXT); Max Planck Society (MPG); Korea Ministry of Education, Science and Technology (MEST)
OSTI Identifier:
1076905
DOE Contract Number:  
AC05-00OR22725
Resource Type:
Journal Article
Journal Name:
Physical Review. B, Condensed Matter and Materials Physics
Additional Journal Information:
Journal Volume: 87; Journal Issue: 13; Journal ID: ISSN 1098-0121
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English

Citation Formats

Fishman, Randy Scott, Haraldsen, Jason T., Furukawa, Nobuo, and Miyahara, Shin. Spin state and spectroscopic modes of multiferroic BiFeO3. United States: N. p., 2013. Web. doi:10.1103/PhysRevB.87.134416.
Fishman, Randy Scott, Haraldsen, Jason T., Furukawa, Nobuo, & Miyahara, Shin. Spin state and spectroscopic modes of multiferroic BiFeO3. United States. https://doi.org/10.1103/PhysRevB.87.134416
Fishman, Randy Scott, Haraldsen, Jason T., Furukawa, Nobuo, and Miyahara, Shin. 2013. "Spin state and spectroscopic modes of multiferroic BiFeO3". United States. https://doi.org/10.1103/PhysRevB.87.134416.
@article{osti_1076905,
title = {Spin state and spectroscopic modes of multiferroic BiFeO3},
author = {Fishman, Randy Scott and Haraldsen, Jason T. and Furukawa, Nobuo and Miyahara, Shin},
abstractNote = {Spectroscopic modes provide the most sensitive probe of the very weak interactions responsible for the properties of the long-wavelength cycloid in the multiferroic phase of BiFeO3 below TN ≈ 640 K. Three of the four modes measured by terahertz (THz) and Raman spectroscopies were recently identified using a simple microscopic model. While a Dzyaloshinskii-Moriya (DM) interaction D along [-1, 2, -1] induces a cycloid with wave vector (2π/α) (0.5 + δ, 0.5, 0.5 - δ) (δ ≈ 0.0045), easy-axis anisotropy K along the [1, 1, 1] direction of the electric polarization P induces higher harmonics of the cycloid, which split the ${\Psi}_{1}$ modes at 2.49 and 2.67 meV and activate the ${{\Phi}}_{2}$ mode at 3.38 meV. However, that model could not explain the observed low-frequency mode at about 2.17 meV. We now demonstrate that an additional DM interaction D' along [1, 1, 1] not only produces the observed weak ferromagnetic moment of the high-field phase above 18 T but also activates the spectroscopic matrix elements of the nearly degenerate, low-frequency ${\Psi}_{0}$ and ${\Phi}_{1}$ modes, although their scattering intensities remain extremely weak. Even in the absence of easy-axis anisotropy, D' produces cycloidal harmonics that split ${\Psi}_{1}$ and activate ${\Phi}_{2}$. However, the observed mode frequencies and selection rules require that both D' and K are nonzero. This work also resolves an earlier disagreement between spectroscopic and inelastic neutron-scattering measurements.},
doi = {10.1103/PhysRevB.87.134416},
url = {https://www.osti.gov/biblio/1076905}, journal = {Physical Review. B, Condensed Matter and Materials Physics},
issn = {1098-0121},
number = 13,
volume = 87,
place = {United States},
year = {2013},
month = {4}
}

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