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Designing high-performance piezoelectric materials based on atomic-scale calculations is highly desired in recent years, following the understanding of the structure-property relationship of state-of-the-art piezoelectric materials. Previous mesoscale simulations showed that local structural heterogeneity plays an important role in the piezoelectric property of ferroelectrics; that is, larger structural heterogeneity leads to higher piezoelectricity. In this Rapid Communication, by combining first-principles calculations and experimental characterizations, we explored the atomic-scale origin of the high piezoelectricity for samarium-doped Pb(Mg1/3Nb2/3)O3-PbTiO3 (PMN-PT) ceramics, which possesses the highest piezoelectric d33 of ∼1500pCN-1 among all known piezoelectric ceramics. The impacts of various dopants on local structure and piezoelectric properties of PMN-PT ceramics were investigated in terms of the effective ionic radius and cation valence. Our results show that A-site dopants with a valence of 3+ are more effective to produce local structural heterogeneity in PMN-PT when compared with the A-site dopants with a valence of 2+, and a smaller dopant size leads to a larger variation of local structure. According to this study, the outstanding piezoelectricity in Sm-doped PMN-PT ceramics is attributed to the fact that Sm3+ is the smallest ions that can entirely go to the A site of PMN-PT rather than the B site. The present work may benefit the design of high-performance piezoelectric materials based on the concept of local structural engineering. Disciplines Engineering | Physical Sciences and Mathematics Publication Details Li, C., Xu, B., Lin, D., Zhang, S., Bellaiche, L., Shrout, T. R. & Li, F. (2020). Atomic-scale origin of ultrahigh piezoelectricity in samarium-doped PMN-PT ceramics. Physical Review B, 101 (14), 140102-1-140102-7. Authors Chunchun Li, Bin Xu, Dabin Lin, Shujun Zhang, Laurent Bellaiche, Thomas R. Shrout, and Fei Li This journal article is available at Research Online: https://ro.uow.edu.au/aiimpapers/4167 PHYSICAL REVIEW B 101, 140102(R) (2020) Rapid Communications Atomic-scale origin of ultrahigh piezoelectricity in samarium-doped PMN-PT ceramics Chunchun Li ,1,2 Bin Xu ,3,4,* Dabin Lin,2 Shujun Zhang ,5 Laurent Bellaiche,4 Thomas R. Shrout,2 and Fei Li 2,6,† 1College of Information Science and Engineering, Guilin University of Technology, Guilin 541004, China 2Materials Research Institute, Pennsylvania State University, University Park, State College, Pennsylvania 168001, USA 3School of Physical Science and Technology, Soochow University, Suzhou, Jiangsu 215006, China 4Natural Science Department of Physics, University of Arkansas, Fayetteville, Arkansas 72701, USA 5Institute for Superconducting and Electronic Materials, Australian Institute for Innovative Materials, University of Wollongong, Wollongong New South Wales 2500, Australia 6Electronic Materials Research Laboratory, Key Laboratory of the Ministry of Education and International Center for Dielectric Research, Xi’an Jiaotong University, Xi’an 710049, China (Received 5 July 2019; revised manuscript received 31 March 2020; accepted 1 April 2020; published 27 April 2020) Designing high-performance piezoelectric materials based on atomic-scale calculations is highly desired in recent years, following the understanding of the structure-property relationship of state-of-the-art piezoelectric materials. Previous mesoscale simulations showed that local structural heterogeneity plays an important role in the piezoelectric property of ferroelectrics; that is, larger structural heterogeneity leads to higher piezoelectricity. In this Rapid Communication, by combining first-principles calculations and experimental characterizations, we explored the atomic-scale origin of the high piezoelectricity for samarium-doped Pb(Mg1/3Nb2/3)O3-PbTiO3 (PMN-PT) ceramics, which possesses the highest piezoelectric d33 of ∼1500 pC N−1 among all known piezoelectric ceramics. The impacts of various dopants on local structure and piezoelectric properties of PMN-PT ceramics were investigated in terms of the effective ionic radius and cation valence. Our results show that A-site dopants with a valence of 3+ are more effective to produce local structural heterogeneity in PMN-PT when compared with the A-site dopants with a valence of 2+, and a smaller dopant size leads to a larger variation of local structure. According to this study, the outstanding piezoelectricity in Sm-doped PMN-PT ceramics is attributed to the fact that Sm3+ is the smallest ions that can entirely go to the A site of PMN-PT rather than the B site. The present work may benefit the design of high-performance piezoelectric materials based on the concept of local structural engineering. DOI: 10.1103/PhysRevB.101.140102