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Ion doping, an effective way to modify the nature of materials, is beneficial for the improvement of material properties. Mn doping exhibits gain of piezoelectric properties in KTa 1- x  Nb  x  O 3 (KTN). However, the impact mechanism of Mn ions on properties remains unclear. Here, the effects of Mn doping on local heterogeneity and piezoelectric properties in KTN are studied. The electric field-induced strain of Mn-doped KTN is ∼0.25% at 10 kV cm -1 , 118% higher than that of pristine KTN. Meanwhile, as a result of Mn doping, the dielectric permittivity was tripled and the ferroelectricity was modified. The changes in A 1 (2TO), B 1 + E(3TO) and E(4TO) vibrations characterized by Raman spectra indicate increased local polarization, weak correlation of dipoles and distorted lattices in Mn-doped KTN, respectively. First-principles calculations demonstrate stronger local heterogeneity introduced by Mn dopants, which weakens the dipole correlations and reduces domain sizes. As a result, the decreased domain sizes, combined with the larger ratio of lattice parameters c and a of the Mn-contained portion, are responsible for the higher piezoelectricity. This work reveals the impact on properties of KTN from Mn dopants and the prominent role of local heterogeneity in improving piezoelectricity, being valuable for the optimization and design of material properties.

Manganese-doping enhanced local heterogeneity and piezoelectric properties in potassium tantalate niobate single crystals