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We report the robust ferroelectric properties of (1 −  x )(Bi 1/2 Na 1/2 )TiO 3 – x (Bi 1/2 K 1/2 )TiO 3  ( x  = 33%) single crystals grown by a top-seeded solution growth process under a high oxygen-pressure (0.9 MPa) atmosphere. The sample exhibit a large remanent polarization of 48 μC/cm 2  and a sizeable piezoelectric strain constant of 460 pm/V. Neutron powder diffraction structural analysis combined with first-principles calculations reveals that the large ferroelectric polarization comparable to PbTiO 3  stems from the hybridization between Bi-6 p  and O-2 p  orbitals at a moderately negative chemical pressure.

Uncovering ferroelectric polarization in tetragonal (Bi1/2K1/2)TiO3–(Bi1/2Na1/2)TiO3 single crystals