Multiferroics are compounds that show ferroelectricity and magnetism. BiFeO3, by far the most studied, has outstanding ferroelectric properties, a cycloidal magnetic order in the bulk, and many unexpected virtues such as conductive domain walls or a low bandgap of interest for photovoltaics. Although this flurry of properties makes BiFeO3 a paradigmatic multifunctional material, most are related to its ferroelectric character, and its other ferroic property—antiferromagnetism—has not been investigated extensively, especially in thin films. Here we bring insight into the rich spin physics of BiFeO3 in a detailed study of the static and dynamic magnetic response of strain-engineered films. Using Mössbauer and Raman spectroscopies combined with Landau–Ginzburg theory and effective Hamiltonian calculations, we show that the bulk-like cycloidal spin modulation that exists at low compressive strain is driven towards pseudo-collinear antiferromagnetism at high strain, both tensile and compressive. For moderate tensile strain we also predict and observe indications of a new cycloid. Accordingly, we find that the magnonic response is entirely modified, with low-energy magnon modes being suppressed as strain increases. Finally, we reveal that strain progressively drives the average spin angle from in-plane to out-of-plane, a property we use to tune the exchange bias and giant-magnetoresistive response of spin valves.
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We are very grateful to D. Colson for providing the 57Fe-enriched target and to P. Bonville, M. A. Méasson, Y. Gallais and S. W. Cheong for stimulating discussions. Financial support from the French Ministère de l’Enseignement Supérieur et de la Recherche, the French Agence Nationale de la Recherche (ANR) through projects NOMILOPS and MULTIDOLLS and the Russian Foundation for Basic Research is acknowledged. D.R. and L.B. thank mostly the support of NSF. They also acknowledge DOE, ARO and ONR for discussions with scientists sponsored by these agencies.
The authors declare no competing financial interests.
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Sando, D., Agbelele, A., Rahmedov, D. et al. Crafting the magnonic and spintronic response of BiFeO3 films by epitaxial strain. Nature Mater 12, 641–646 (2013). https://doi.org/10.1038/nmat3629
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