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Understanding the depolarization of ferroelectric materials caused by external stimuli is critical for maintaining the aligned polarization states. Although thermal depolarization in poled materials is well established, the mechanisms of electric field-induced depolarization remain largely unexplored. In this study, we investigate the electrical depoling behavior of [001]-oriented rhombohedral Pb(Mg1/3Nb2/3)O3-PbTiO3 (PMN-PT) single crystals poled using direct current poling (DCP) and alternating current poling (ACP). We reveal that the ACP sample exhibits a lower reverse coercive field than the DCP specimen. We compare the effects of bipolar and unipolar electric fields applied in the reverse poling direction, analyzing the changes in permittivity and piezoelectric resonance. Piezoresponse force microscopy is employed to characterize domain configurations in poled and electrically depoled samples. Our findings suggest that property degradation may arise from the nucleation and growth of domains oriented opposite to the initial arrangement. 

Abstract The understanding of domain dynamics in ferroelectric materials is crucial for optimizing their performance in piezoelectric and electro‐optic applications. Although previous studies have focused on static domain structures and macroscopic characteristics, the time‐resolved approach of domains remains largely unexplored. In this study, we compare the dynamic responses of direct current (DC) and alternating current (AC) poled [001]‐oriented rhombohedral Pb(Mg_1/3Nb_2/3)O₃–PbTiO₃(PMN–PT) single crystals using X‐ray photon correlation spectroscopy (XPCS) during the application of external electric fields. Our results demonstrate that the AC‐poled sample exhibit enhanced reconfiguration of domain variants in response to driving fields compared to the DC‐poled counterpart, as evidenced by accelerated correlation decay and faster relaxation time. This phenomenon is attributed to enhanced reversible domain wall motion achieved through AC poling, which facilitates field‐induced domain realignment. These findings provide insight into the relationship between dynamics and macroscopic properties in relaxor‐PT single crystals for high‐performance applications.