Department of Materials Science & Engineering, University of Wisconsin-Madison , Madison, Wisconsin 53706, United States.
Department of Chemical & Biological Engineering, University of Wisconsin-Madison , Madison, Wisconsin 53706, United States.
ACS Appl Mater Interfaces. 2017 Nov 22;9(46):41034-41042. doi: 10.1021/acsami.7b12978. Epub 2017 Nov 13.
Integration of emerging complex-oxide compounds into sophisticated nanoscale single-crystal geometries faces significant challenges arising from the kinetics of vapor-phase thin-film epitaxial growth. A comparison of the crystallization of the model perovskite SrTiO (STO) on (001) STO and oxidized (001) Si substrates indicates that there is a viable alternative route that can yield three-dimensional epitaxial synthesis, an approach in which STO is crystallized from an amorphous thin film by postdeposition annealing. The crystallization of amorphous STO on single-crystal (001) STO substrates occurs via solid-phase epitaxy (SPE), without nucleation and with a temperature-dependent amorphous/crystalline interface velocity. In comparison, the crystallization of STO on SiO/(001) Si substrates requires nucleation, resulting in a polycrystalline film with crystal sizes on the order of 10 nm. A comparison of the temperature dependence of the nucleation and growth processes for these two substrates indicates that it will be possible to create crystalline STO materials using low-temperature crystallization from a crystalline seed, even in the presence of interfaces with other materials. These processes provide a potential route for the formation of single crystals with intricate three-dimensional nanoscale geometries.
新兴的复杂氧化物化合物与复杂的纳米级单晶结构的集成面临着来自气相薄膜外延生长动力学的重大挑战。对模型钙钛矿 SrTiO(STO)在(001) STO 和氧化(001) Si 衬底上的结晶的比较表明,存在一种可行的替代途径,可以实现三维外延合成,这种方法是通过沉积后退火使 STO 从非晶薄膜中结晶。非晶 STO 在单晶(001) STO 衬底上的结晶通过固相外延(SPE)发生,没有成核且具有与温度相关的非晶/晶界速度。相比之下, STO 在 SiO/(001) Si 衬底上的结晶需要成核,导致具有约 10nm 量级的晶粒尺寸的多晶膜。对这两种衬底上的成核和生长过程的温度依赖性的比较表明,即使存在与其他材料的界面,也可以使用低温从晶种结晶来制造结晶 STO 材料。这些过程为具有复杂三维纳米级几何形状的单晶的形成提供了一种潜在途径。