Functional oxides on silicon have been the subject of in-depth research for more than 20 years. Much of this research has been focused on the quality of the integration of materials due to their intrinsic thermodynamic incompatibility, which has hindered the flourishing of the field of research. Nevertheless, growth of epitaxial transition metal oxides on silicon with a sharp interface has been achieved by elaborated kinetically controlled sequential deposition while the crystalline quality of different functional oxides has been considerably improved. In this Research Update, we focus on three applications in which epitaxial ferroelectric oxides on silicon are at the forefront, and in each of these applications, other aspects of the integration of materials play an important role. These are the fields of piezoelectric microelectromechanical system devices, electro-optical components, and catalysis. The overview is supported by a brief analysis of the synthesis processes that enable epitaxial growth of oxides on silicon. This Research Update concludes with a theoretical description of the interfaces and the possibility of manipulating their electronic structure to achieve the desired coupling between (ferroelectric) oxides and semiconductors, which opens up a remarkable perspective for many advanced applications.

The application of two-dimensional (2D) materials has alleviated a number of challenges of traditional epitaxy and pushed forward the integration of dissimilar materials. Besides acting as a seed layer for van der Waals epitaxy, the 2D materials� being atom(s) thick�have also enabled wetting transparency in which the potential field of the substrate, although partially screened, is still capable of imposing epitaxial overgrowth. One of the crucial steps in this technology is the preservation of the quality of 2D materials during and after their transfer to a substrate of interest. In the present study, we show that by honing the achievements of traditional epitaxy and wet chemistry a hybrid approach can be devised that offers a unique perspective for the integration of functional oxides with a silicon platform. It is based on SrO-assisted deoxidation and controllable coverage of silicon surface with a layer(s) of spin-coated graphene oxide, thus simultaneously allowing both direct and van der Waals epitaxy of SrTiO 3 (STO). We were able to grow a high-quality STO pseudosubstrate suitable for further overgrowth of functional oxides, such as PbZr 1−x Ti x O 3 (PZT). Given that the quality of the films grown on a reduced graphene oxide-buffer layer was almost identical to that obtained on SiC-derived graphene, we believe that this approach may provide new routes for direct and "remote" epitaxy or layer-transfer techniques of dissimilar material systems.

The study of oxide electrocatalysts is often complicated by the formation of complex and unknown surface species as well as the interaction between the catalysts and common support materials. Because...

Envisioned extremely scaled, high-performance memory devices request to conduct the step from thin semiconductor films to nanoscale structures and the use of promising high-k materials such as hafnium oxide (HfO 2 ). HfO 2 is well suited for use in resistive random-access memory (ReRAM) devices based on the valence change mechanism. Here, we provide a decidedly scaled system, namely, HfO 2 nanoislands that are grown by van der Waals epitaxy on highly oriented pyrolytic graphite (HOPG). The electronic and structural properties of these wellseparated, crystalline HfO 2 nanoislands are investigated by scanning probe methods as well as ab initio methods. The topography reveals homogeneously formed HfO 2 nanoislands with areas down to 7 nm 2 and a thickness of one unit cell. They exhibit several acceptor-and donor-like in-gap states in addition to the bulk band gap, implying bulk properties. X-ray photoelectron spectroscopy indicates hafnium carbide formation as one possible origin for defect states. Going further to the crystal nucleation of HfO 2 , nanocrystals with a diameter of 2.7−4.5 Å are identified next to carbon vacancies in the topmost HOPG layer, indicating that carbon is incorporated into the islands at early nucleation stages. A precise description of these nuclei is accomplished by the simulation of small Hf m O n (:C) clusters (m = 3 to 10; n = 3 to 22) with and without carbon incorporation using ab initio methods. The comparison of the theoretically determined lowest-energy clusters and electronic states with the experimental results allows us to identify the structure of the most relevant HfO 2 sub-nanometer crystals formed during the first nucleation steps and the nature of the in-gap states found at the surfaces of HfO 2 nanoislands. That way, a model system is derived that consists of distinct structural units, related to surface states or defect states, respectively, that will promote the tailoring of in-gap states of smallest HfO 2 structures and thus the scalability of memory devices.

Understanding the relationship between structural characteristics and functional properties of complex relaxor ferroelectric thin films is of high interest for designing materials with high performances. In this work, the structure of epitaxial relaxed pulsed-laser-deposited Pb(Mg1/3Nb2/3)O3-xPbTiO3 (PMN-xPT; x = 25, 33, and 40) thin films on LaNiO3/SrTiO3 substrates is analyzed using a variety of diffraction and spectroscopic techniques. While based on the data obtained from high-resolution x-ray diffraction and scanning transmission electron microscopy analysis, the average structure of the PMN-xPT films is metrically cubic, micro-Raman polarimetry measurements indicate the tetragonal-like ferroelectric phase with marked preference for the polarization perpendicular to the film for all three compositions. The results of the Raman scattering analysis are supported by electromechanical properties of the samples, which clearly show that the films have a locally non-centrosymmetric structure. Furthermore, only a gradual enhancement of the electrical properties from PMN-25PT to PMN-40PT is observed, which is attributed to small tetragonal distortions that are highly similar for all three compositions.