Temperature-Dependent Domain Dynamics and Electrical Properties of Nd-doped Bi4Ti2.99Mn0.01O12 Thin Films in Fatigue Process

Bi4Ti2.99Mn0.01O12 (BTM) thin films with different ratio of neodymium (Nd) doping were prepared on Pt(111)/Ti/SiO2/Si(100) substrates through a sol-gel method. The effects of Nd doping on domain dynamics and temperature-dependent fatigue behaviors of BTM thin films were systematically studied. The polarization fatigues of BTM (not doped) and Bi3.5Nd0.5Ti2.99Mn0.01O12 (BNTM05) thin films first get better with the increasing temperature (T) from 300 to 350 K and then become worse from 350 to 400 K, while Bi3.15Nd0.85Ti2.99Mn0.01O12 (BNTM85) thin films show enhanced fatigue endurance from 300 to 400 K. It can be shown that the long-range diffusion of oxygen vacancies in BTM thin film happens more easily through the impedance spectra analysis with T from 300 to 475 K, which can be verified by a lower activation energies (0.13–0.14 eV) compared to those of BNTM05 and BNTM85 (0.17–0.21 eV). Using a temperature-dependent piezoresponse force microscopy (PFM), we have found more responsive domain fragments in Nd-substituted films. The microscopic domain evolution from 298 to 448 K was done to further explain that the domain wall unpinning effect has been enhanced with increasing T. The correlation between microscopic domain dynamics and macroscopic electrical properties clearly demonstrates the effects of charged domain wall in Nd-doped BTM thin films during the fatigue tests.