- Xu, Ruijuan;
- Crust, Kevin J;
- Harbola, Varun;
- Arras, Rémi;
- Patel, Kinnary Y;
- Prosandeev, Sergey;
- Cao, Hui;
- Shao, Yu‐Tsun;
- Behera, Piush;
- Caretta, Lucas;
- Kim, Woo Jin;
- Khandelwal, Aarushi;
- Acharya, Megha;
- Wang, Melody M;
- Liu, Yin;
- Barnard, Edward S;
- Raja, Archana;
- Martin, Lane W;
- Gu, X Wendy;
- Zhou, Hua;
- Ramesh, Ramamoorthy;
- Muller, David A;
- Bellaiche, Laurent;
- Hwang, Harold Y
Despite extensive studies on size effects in ferroelectrics, how structures and properties evolve in antiferroelectrics with reduced dimensions still remains elusive. Given the enormous potential of utilizing antiferroelectrics for high-energy-density storage applications, understanding their size effects will provide key information for optimizing device performances at small scales. Here, the fundamental intrinsic size dependence of antiferroelectricity in lead-free NaNbO3 membranes is investigated. Via a wide range of experimental and theoretical approaches, an intriguing antiferroelectric-to-ferroelectric transition upon reducing membrane thickness is probed. This size effect leads to a ferroelectric single-phase below 40 nm, as well as a mixed-phase state with ferroelectric and antiferroelectric orders coexisting above this critical thickness. Furthermore, it is shown that the antiferroelectric and ferroelectric orders are electrically switchable. First-principle calculations further reveal that the observed transition is driven by the structural distortion arising from the membrane surface. This work provides direct experimental evidence for intrinsic size-driven scaling in antiferroelectrics and demonstrates enormous potential of utilizing size effects to drive emergent properties in environmentally benign lead-free oxides with the membrane platform.