Quantitative biaxial texture analysis with reflection high-energy electron diffraction for ion beam-assisted deposition of MgO and heteroepitaxy of perovskite ferroelectrics

Abstract

To facilitate ferroelectric-based actuator integration with silicon electronics fabrication technology, we have developed a route to produce biaxially textured ferroelectrics on amorphous layers by using biaxially textured MgO templates. Using a kinematical electron scattering model, we show that the RHEED pattern from a biaxially textured polycrystalline film can be calculated from an analytic solution to the electron scattering probability. We found that diffraction spot shapes are sensitive to out-of-plane orientation distributions and in-plane RHEED rocking curves are sensitive to the in-plane orientation distribution. Using information from the simulation, a RHEED-based experimental technique was developed for in situ measurement of MgO biaxial texture. The accuracy of this technique was confirmed by comparing RHEED measurements of in-plane and out-of-plane orientation distribution with synchrotron x-ray rocking curve measurements. Biaxially textured MgO was grown on amorphous Si3N4 by ion beam-assisted deposition (IBAD). MgO was e-beam evaporated onto the amorphous substrate with a simultaneous 750-1200 eV Ar+ ion bombardment at 45o from normal incidence. We observed a previously unseen, dramatic texture evolution in IBAD MgO using transmission electron microscopy (TEM) and RHEED-based quantitative texture measurements of MgO. The first layers of IBAD MgO are diffraction amorphous until the film is about 3.5 nm thick. During the next 1 nm of additional growth, we observed rapid biaxial texture evolution. RHEED and TEM studies indicate that biaxially textured MgO film results from a solid phase crystallization of biaxially textured MgO crystals in an amorphous matrix. Biaxially textured perovskite ferroelectrics were grown on biaxially textured MgO templates using sol-gel, metallorganic chemical vapor deposition (MOCVD), and molecular beam epitaxy (MBE). Through RHEED-based biaxial texture analysis we observed that the heteroepitaxial ferroelectric in-plane orientation distribution, deposited using ex situ techniques (not performed in the same high vacuum growth environment where the MgO was deposited), narrowed significantly with respect to the in-plane orientation distribution of its MgO template (from 11o to 6o FWHM). Evidence from cross section TEM and RHEED suggest that atmospheric moisture degrades the crystallinity of highly defective, misaligned MgO grains and that heteroepitaxially grown ferroelectrics preferentially nucleate on well-aligned grains and over grow misaligned regions of MgO.