In this work, the piezoelectric and dielectric properties of [001]-oriented 0.7Pb(Mg1/3Nb2/3)O3-0.3PbTiO3 single crystals under alternating current poling (ACP) at different temperatures were studied. The piezoelectric coefficients (d33 ∼ 1930 pC/N, d31 ∼ −850 pC/N) and free dielectric permittivity (εT33/ε0 ∼ 7570) reached their highest values when the poling temperature (Tpoling) was 70 °C. Compared with traditional direct current electric field poling at 20 °C, 70 °C-ACP samples showed an enhancement of 40%, 35%, and 49% for d33, d31, and εT33/ε0, respectively. Meanwhile, d33 and εT33/ε0 were enhanced by about 9% when Tpoling increased from 20 °C to 70 °C under ACP, while d31 remained the same value and the dielectric loss was lowered from 0.29% to 0.22%. Moreover, ACP samples with different Tpoling have similar electromechanical coupling factors (k31 ∼ 0.44, kt ∼ 0.60). A discussion of the mechanism for the ACP enhancement was based on the domain observation using piezoresponse force microscopy, and the results showed that the domain densities of ACP samples with different Tpoling were positively correlated with their piezoelectric properties. This work demonstrated the enormous potential of ACP optimization for relaxor-PT single crystal applications.

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Alternating current poling (ACP) was performed on Gen III relaxor-PT Mn-doped Pb(In1/2Nb1/2)O3-Pb(Mg1/3Nb2/3)O3-PbTiO3 (Mn: PIN-PMN-PT) single crystals with the poling direction of [001]. Experimental results proved that ACP could bring property enhancement to both k31 and k33 mode crystals. Compared to those from traditional direct current poling (DCP), ACP with the optimized conditions (20 kV/cm, 0.1 Hz, and 20 cycles) enhanced the dielectric and piezoelectric properties of k31-mode mode crystals by more than 30%, where the enhanced free dielectric constant and piezoelectric coefficient d33 reached 5300 and 1750 pC/N, respectively. Furthermore, replacing DCP with ACP could increase the advantages of Gen III relaxor-PT. The coupling factors k31 and k33 were enhanced to 0.472 and 0.915, the mechanical quality factor Qm was enhanced by 17%, and the depoling temperature was raised by 17 °C to 123 °C. In the following mechanism study, in situ x-ray diffraction (XRD) combined with the temperature-dependent dielectric constant measurement proved the introduction of the monoclinic phases after ACP, while piezoresponse force microscopy (PFM) observation showed “2R”-like “2M” domain morphologies in ACP single crystals. Both these intrinsic and extrinsic factors are believed to be the keys to the mechanisms of property enhancement behind ACP. This study proved that ACP is an effective property enhancement method suitable for Gen III relaxor-PT single crystals and will promote its applications in high-temperature and high-power devices.

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Alternating current (electric field) poling (ACP) was applied on [001]-oriented 0.7Pb(Mg1/3Nb2/3)O3-0.3PbTiO3 (PMN-0.3PT) single crystal samples with dimensions of 5 × 1.25 × 1.25 mm3 (with electrodes on the 1.25 × 1.25 mm2 surfaces), and the influence of ACP frequency (fACP) was studied. Compared to those from traditional direct (electric field) poling samples, the piezoelectric coefficient (d33) and free dielectric constant (εT33/ε0) of ACP samples could gain up to a 67% increase to 3200 pC/N and 10 500, respectively. The influence of fACP was studied on two main aspects: saturated properties and dynamic saturation process. In general, ACP samples with lower fACP had higher saturated d33, εT33/ε0, and coupling factor k33, as well as lower dielectric loss and faster saturation speed. The ACP dynamics during the saturation process were studied by measuring the polarization-vs-electric field hysteresis loops (P-E loops). The P-E loops illustrated that the coercive field of ACP samples could be further tuned from 1.84 kV/cm to 3.03 kV/cm by changing fACP (0.1–10 Hz). This work demonstrated the enormous potential of ACP optimization in relaxor-PT single crystal-based low-frequency transducer applications.