Magnon sidebands and spin-charge coupling in bismuth ferrite probed by nonlinear optical spectroscopy

M. O. Ramirez, A. Kumar, S. A. Denev, N. J. Podraza, X. S. Xu, R. C. Rai, Y. H. Chu, J. Seidel, L. W. Martin, S.-Y. Yang, E. Saiz, J. F. Ihlefeld, S. Lee, J. Klug, S. W. Cheong, M. J. Bedzyk, O. Auciello, D. G. Schlom, R. Ramesh, J. Orenstein, J. L. Musfeldt, and V. Gopalan
Phys. Rev. B 79, 224106 – Published 5 June 2009
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Abstract

The interplay between spin waves (magnons) and electronic structure in materials leads to the creation of additional bands associated with electronic energy levels which are called magnon sidebands. The large difference in the energy scales between magnons (meV) and electronic levels (eV) makes this direct interaction weak and hence makes magnon sidebands difficult to probe. Linear light absorption and scattering techniques at low temperatures are traditionally used to probe these sidebands. Here we show that optical second-harmonic generation, as the lowest-order nonlinear process, can successfully probe the magnon sidebands at room temperature and up to 723 K in bismuth ferrite, associated with large wave vector multimagnon excitations which linear absorption studies are able to resolve only under high magnetic fields and low temperatures. Polarized light studies and temperature dependence of these sidebands reveal a spin-charge coupling interaction of the type PsL2 between the spontaneous polarization (Ps) and antiferromagnetic order parameter, L in bismuth ferrite, that persists with short-range correlation well into the paramagnetic phase up to high temperatures. These observations suggest a broader opportunity to probe the collective spin-charge-lattice interactions in a wide range of material systems at high temperatures and electronic energy scales using nonlinear optics.

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  • Received 22 January 2009

DOI:https://doi.org/10.1103/PhysRevB.79.224106

©2009 American Physical Society

Authors & Affiliations

M. O. Ramirez1, A. Kumar1, S. A. Denev1, N. J. Podraza1,2, X. S. Xu3, R. C. Rai3, Y. H. Chu4,5, J. Seidel4,5, L. W. Martin4, S.-Y. Yang4, E. Saiz4, J. F. Ihlefeld2,4, S. Lee6, J. Klug7,8, S. W. Cheong6, M. J. Bedzyk7,8, O. Auciello8, D. G. Schlom1, R. Ramesh4,5, J. Orenstein5, J. L. Musfeldt3, and V. Gopalan1

  • 1Department of Materials Science and Engineering and Materials Research Institute, Pennsylvania State University, University Park, Pennsylvania 16802, USA
  • 2Department of Electrical Engineering and Materials Research Institute, Pennsylvania State University, University Park, Pennsylvania 16802, USA
  • 3Department of Chemistry, University of Tennessee, Knoxville, Tennessee 37996, USA
  • 4Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, USA
  • 5Department of Physics, University of California, Berkeley, California 94720-1760, USA
  • 6Department of Physics and Astronomy Rutgers and Rutgers Center of Emergent Materials, The State University of New Jersey, 136 Frelinghuysen Road, Piscataway, New Jersey 08854-8019, USA
  • 7Materials Research Center, Northwestern University, Evanston, Illinois 60208, USA
  • 8Materials Science Division, Argonne National Laboratory, Argonne, Illinois 60439, USA

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Issue

Vol. 79, Iss. 22 — 1 June 2009

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