Abstract Lead‐based relaxor ferroelectrics are characterized by outstanding piezoelectric and dielectric properties, making them useful in a wide range of applications. Despite the numerous models proposed to describe the relation between their nanoscale polar structure and the large properties, the multiple contributions to these properties are not yet revealed. Here, by combining atomistic and mesoscopic‐scale structural analyses with macroscopic piezoelectric and dielectric measurements across the (100–x)Pb(Mg1/3Nb2/3)O3–xPbTiO3(PMN–xPT) phase diagram, a direct link is established between the multiscale structure and the large nonlinear macroscopic response observed in the monoclinic PMN‐xPT compositions. The approach reveals a previously unrecognized softening effect, which is common to Pb‐based relaxor ferroelectrics and arises from the displacements of low‐angle nanodomain walls, facilitated by the nanoscale polar character and lattice strain disorder. This comprehensive comparative study points to the multiple, distinct mechanisms that are responsible for the large piezoelectric response in relaxor ferroelectrics. 
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                            Heterogeneous field response of hierarchical polar laminates in relaxor ferroelectrics
                        
                    
    
            Understanding the microscopic origin of the superior electromechanical response in relaxor ferroelectrics requires knowledge not only of the atomic-scale formation of polar nanodomains (PNDs) but also the rules governing the arrangements and stimulated response of PNDs over longer distances. Using x-ray coherent nanodiffraction, we show the staggered self-assembly of PNDs into unidirectional mesostructures that we refer to as polar laminates in the relaxor ferroelectric 0.68PbMg1/3Nb2/3O3-0.32PbTiO3(PMN-0.32PT). We reveal the highly heterogeneous electric-field–driven responses of intra- and interlaminate PNDs and establish their correlation with the local strain and the nature of the PND walls. Our observations highlight the critical role of hierarchical lattice organizations on macroscopic material properties and provide guiding principles for the understanding and design of relaxors and a wide range of quantum and functional materials. 
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                            - Award ID(s):
- 2329111
- PAR ID:
- 10534629
- Publisher / Repository:
- AAAS
- Date Published:
- Journal Name:
- Science
- Volume:
- 384
- Issue:
- 6703
- ISSN:
- 0036-8075
- Page Range / eLocation ID:
- 1447-1452
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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