The effect of MnO 2 addition on the dielectric and piezoelectric properties of 0.4Pb͑Mg 1/3 Nb 2/3 ͒O 3 -0.25PbZrO 3 -0.35PbTiO 3 single crystals was investigated. Analogous to acceptor doping in "hard" Pb͑Zr, Ti͒O 3 based polycrystalline materials, the Mn doped crystals exhibited enhanced mechanical Q ͑ϳ1050͒ with low dielectric loss ͑ϳ0.2% ͒, while maintaining ultrahigh electromechanical coupling k 33 Ͼ 90%, inherent in domain engineered single crystals. The effect of acceptor doping was also evident in the build-up of an internal bias ͑E i ϳ 1.6 kV/ cm͒, shown by a horizontal offset in the polarization-field behavior. Together with the relatively high usage temperature ͑T R-T ϳ 140°C͒, the Mn doped crystals are promising candidates for high power and broad bandwidth transducers. © 2008 American Institute of Physics. ͓DOI: 10.1063/1.2992081͔High power ultrasonic transducers generally use "hard" piezoelectric ceramics Pb͑Zr, Ti͒O 3 ͑PZT͒, including PZT4 and PZT8 ͑DOD types I and III͒ 1 . These materials are characterized by low dielectric ͑tan ␦͒ and mechanical losses ͑high mechanical quality factor Q͒. In general, to achieve the "hardening" effect, these materials are acceptor doped, e.g., Fe 3+,2+ , Mn 3+,2+ substitution for Zr 4+ / Ti 4+ , resulting in the development of acceptor-oxygen vacancy defect dipoles. These dipoles align parallel to the polarization direction, leading to an internal bias, as evident in a horizontal offset in the polarization-electric field ͑P-E͒ behavior. This offset effectively increases the coercive field ͑E C ͒ and reduces or clamps domain wall motion/mobility. 2,3 A consequence of these dopants, however, is a reduction in electromechanical coupling and piezoelectric activity, with k 33 values less than 70% and piezoelectric strain coefficients d 33 's on the order of 200-350 pC/ N, 4 so limits the bandwidth of transducer since the power and bandwidth capabilities of the transducer are functions of the mechanical quality and electromechanical coupling factors 5,6 . Recently, domain engineered ͗001͘ oriented single crystal perovskites have been demonstrated to possess ultrahigh electromechanical couplings k 33 Ͼ 90% and high piezoelectric coefficients d 33 Ͼ 1500 pC/ N. However, the relaxor-PbTiO 3 ͑PT͒ crystals exhibit low mechanical quality Q's ͑Ͻ100͒ and coercive fields ͑E C ϳ 2-3 kV/ cm͒, typical of "soft" piezoelectric behavior. 7-9 Numerous efforts have been made to piezoelectrically harden the crystals through the addition of acceptor dopants. To date, only moderate mechanical Q values in the range of 200-300 have been achieved in flux grown Pb͑Zn 1/3 Nb 2/3 ͒O 3 -PbTiO 3 crystals. [10][11][12] In this work, the effect of acceptor doping with MnO 2 in solid state crystal grown ͑SSCG͒ 0.4Pb͑Mg 1/3 Nb 2/3 ͒O 3 -0.25PbZrO 3 -0.35PbTiO 3 ͑PMN-PZT͒ crystals was investigated. The SSCG method was selected owing to its inherent benefit of maintaining dopant uniformity in a solid solution, unlike the melt Bridgman process. The PMN-PZT composition was selected owing to its relatively...