Two-phonon coupling to the antiferromagnetic phase transition in multiferroic BiFeO3
Mariola O. Ramirez, M. Krishnamurthi, S. Denev, A. Kumar, Seung-Yeul, Yang, Ying-Hao Chu, Eduardo Saiz, Jan Seidel, A.P Pyatakov, A.Bush, D., Viehland, J. Orenstein, R. Ramesh, Venkatraman Gopalan

TL;DR
This study reports a two-phonon Raman scattering band in BiFeO3 that exhibits a strong anomaly at the antiferromagnetic transition temperature, revealing significant spin-phonon coupling in this multiferroic material.
Contribution
It demonstrates the direct coupling between two-phonon Raman modes and the antiferromagnetic phase transition in BiFeO3, highlighting a new aspect of spin-lattice interactions.
Findings
The 2E8 Raman mode nearly disappears at the Neel temperature.
A prominent two-phonon band is observed at 1000-1300 cm-1.
Strong anomaly in the two-phonon band at the magnetic transition.
Abstract
A prominent band centered at around 1000-1300 cm-1 and associated with resonant enhancement of two-phonon Raman scattering is reported in multiferroic BiFeO3 thin films and single crystals. A strong anomaly in this band occurs at the antiferromagnetic Neel temperature. This band is composed of three peaks, assigned to 2A4, 2E8, and 2E9 Raman modes. While all three peaks were found to be sensitive to the antiferromagnetic phase transition, the 2E8 mode, in particular, nearly disappears at TN on heating, indicating a strong spin-two phonon coupling in BiFeO3.
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