Freestanding crystalline oxide perovskites down to the monolayer limit

• Published in: Nature (London) 2019-06, Vol.570 (7759), p.87-90
• Main Authors: Ji, Dianxiang, Cai, Songhua, Paudel, Tula R., Sun, Haoying, Zhang, Chunchen, Han, Lu, Wei, Yifan, Zang, Yipeng, Gu, Min, Zhang, Yi, Gao, Wenpei, Huyan, Huaixun, Guo, Wei, Wu, Di, Gu, Zhengbin, Tsymbal, Evgeny Y., Wang, Peng, Nie, Yuefeng, Pan, Xiaoqing
• Format: Article
• Language: English
• Subjects: 639/301/357/1018; 639/766/119/544; 639/766/119/996; Analysis; Bismuth compounds; Carbon; Correlation; Crystal structure; Crystallinity; Fabrication; Ferroelectrics; Graphene; Humanities and Social Sciences; Letter; Materials; Metal oxides; Molecular beam epitaxy; Monolayers; Monomolecular films; multidisciplinary; Oxide coatings; Perovskite; Perovskites; Phase transitions; Phases; Polyethylene terephthalate; Quality; Science; Science & Technology - Other Topics; Science (multidisciplinary); Silicon substrates; Silicon wafers; Strontium titanates; Structure; Thickness; Thin films; Transition metal compounds; Transition metal oxides; Two dimensional materials; Unit cell
• ISSN: 0028-0836; 1476-4687
• DOI: 10.1038/s41586-019-1255-7

Two-dimensional (2D) materials such as graphene and transition-metal dichalcogenides reveal the electronic phases that emerge when a bulk crystal is reduced to a monolayer 1 – 4 . Transition-metal oxide perovskites host a variety of correlated electronic phases 5 – 12 , so similar behaviour in monolayer materials based on transition-metal oxide perovskites would open the door to a rich spectrum of exotic 2D correlated phases that have not yet been explored. Here we report the fabrication of freestanding perovskite films with high crystalline quality almost down to a single unit cell. Using a recently developed method based on water-soluble Sr 3 Al 2 O 6 as the sacrificial buffer layer 13 , 14 we synthesize freestanding SrTiO 3 and BiFeO 3 ultrathin films by reactive molecular beam epitaxy and transfer them to diverse substrates, in particular crystalline silicon wafers and holey carbon films. We find that freestanding BiFeO 3 films exhibit unexpected and giant tetragonality and polarization when approaching the 2D limit. Our results demonstrate the absence of a critical thickness for stabilizing the crystalline order in the freestanding ultrathin oxide films. The ability to synthesize and transfer crystalline freestanding perovskite films without any thickness limitation onto any desired substrate creates opportunities for research into 2D correlated phases and interfacial phenomena that have not previously been technically possible. Ultrathin freestanding crystalline films of transition-metal oxide perovskites are fabricated and transferred to various substrates, proving their potential for exploring emergent 2D correlated phases.