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By performing first-principles calculations, we systematically explore theeffect of epitaxial strain on the structure and properties of multiferroicTbMnO3. We show that, although the unstrained bulk TbMnO3 displays anon-collinear antiferromagnetic spin order, TbMnO3 can be ferromagnetic undercompressive strain, in agreement with the experimental results on TbMnO3 grownon SrTiO3. By increasing the tensile strain up to 5%, we predict that TbMnO3transforms into a new multiferroic state with a large ferroelectricpolarization,two orders of magnitude larger than that in the unstrained bulk,and with a relatively high Neel temperature E-type antiferromagnetic order. Wealso find that the ferroelectric domain and antiferromagnetic domain areinterlocked with each other, thus an external electric field can switch theferroelectric domain and the antiferromagnetic domain simultaneously. Our workdemonstrates that strain engineering can be used to improve the multiferroicproperties of TbMnO3.

A New Multiferroic State with Large Electric Polarization in Tensile Strained TbMnO3