We report on growth-mode transitions in the growth of SrRuO 3 thin films on atomically flat Ti 4+ single-terminated SrTiO 3 (111) substrates, investigated by reflection high-energy electron diffraction and atomic force microscopy. Over the first ~9 unit cells, the dominant growth mode changes from island to layer-by-layer for the growth rate of 0.074 unit cells/sec and the growth temperature of 700 ºC. Moreover, in the course of growing SrRuO 3 films, the governing growth mode of interest can be manipulated by changing the growth temperature and the growth rate, which change allows for the selection of the desired layer-by-layer mode. The present study thus paves the way for integrations of SrRuO 3 thin layers into (111)-orientated oxide heterostructures, and hence multi-functional devices, requiring control of the sharp atomic-level interfaces and the layer-by-layer growth mode.
a)Author to whom all correspondence should be addressed. E-mail: sangkoog@snu.ac.kr 1 Controlling the crystallographic orientation of thin films by altering that of a substrate on which the films are grown has been one of the pursuits for fabrications of oxide heterostructures of new and better physical properties. For instance, a manipulation of a nearest neighbor atomic ordering through an alternate stacking of one unit-cell layers in two perovskite oxides on (111)-oriented substrates has been theoretically predicted to lead to a different magnetic ordered state, which would not be observed from bulk materials. 1 In addition, such ferroelectric oxide films as SrBi 2 Nb 2 O 9 and BiFeO 3 , which would not be polar-axis oriented on (001)-oriented substrates, have exhibited enhanced spontaneous electric polarizations when they are grown on (111)-oriented substrates. 2,3 Not only as a ferromagnetic functional component in (111)-oriented functional heteroepitaxial devices, but an electrode in (111)-oriented ferroelectric capacitors, free from fatigue and imprinting behaviors, SrRuO 3 (SRO) thin films would be one of promising candidates to be integrated into such (111)-oriented structures, as have been favorably integrated into (001)-oriented heterostructures. 4,5 The key to realizing (111)-oriented oxide heterosturctures is the control of sharp heterointerfaces on the atomic level, and thus the control of a favorable growth mode, the so-called layer-by-layer growth mode is prerequisite. Despite such a strong need for (111)-oriented oxide heterostructures, realizing the layer-by-layer growth of SRO films on SrTiO 3 (STO) (111) has yet to be reported because an atomically well-defined, single-2 terminated STO (111) surface has proved difficult to achieve. A recent accomplishment of successful fabrications of such a STO (111) surface by Chang et al.,6 however, has opened the door to the layer-by-layer growth of SRO thin films, enabling SRO thin films to be integrated into (111)-oriented oxide heterostructures.In this letter, we report on anomalous growth-mode transitions at the initial growth of SRO thin films on single-terminated ST...