- Damodaran, Anoop R;
- Pandya, Shishir;
- Agar, Josh C;
- Cao, Ye;
- Vasudevan, Rama K;
- Xu, Ruijuan;
- Saremi, Sahar;
- Li, Qian;
- Kim, Jieun;
- McCarter, Margaret R;
- Dedon, Liv R;
- Angsten, Tom;
- Balke, Nina;
- Jesse, Stephen;
- Asta, Mark;
- Kalinin, Sergei V;
- Martin, Lane W
Leveraging competition between energetically degenerate states to achieve large field-driven responses is a hallmark of functional materials, but routes to such competition are limited. Here, a new route to such effects involving domain-structure competition is demonstrated, which arises from strain-induced spontaneous partitioning of PbTiO3 thin films into nearly energetically degenerate, hierarchical domain architectures of coexisting c/a and a1 /a2 domain structures. Using band-excitation piezoresponse force microscopy, this study manipulates and acoustically detects a facile interconversion of different ferroelastic variants via a two-step, three-state ferroelastic switching process (out-of-plane polarized c+ → in-plane polarized a → out-of-plane polarized c- state), which is concomitant with large nonvolatile electromechanical strains (≈1.25%) and tunability of the local piezoresponse and elastic modulus (>23%). It is further demonstrated that deterministic, nonvolatile writing/erasure of large-area patterns of this electromechanical response is possible, thus showing a new pathway to improved function and properties.