We employed in situ Raman spectroscopy under electric field for (100)/(001)-oriented tetragonal Pb (Ti0.61 Zr0.39) O 3 films with (001)-volume fraction (VC) of 35%. The increase in VC was revealed above 200 kV/cm, which resulted in the larger remanent polarization. In addition, the application of high enough field also brings a feature, i.e., large reversible change in VC with/without electric field that can quantitatively explain the enhanced piezoelectric response. These demonstrate the usefulness of in situ Raman observation to probe the domain contributions to the electrical and piezoelectric responses.
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