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Hybrid molecular beam epitaxy (MBE) growth of Sn-modified BaTiO3 films was realized with varying domain structures and crystal symmetries across the entire composition space. Macroscopic and microscopic structures and the crystal symmetry of these thin films were determined using a combination of optical second harmonic generation (SHG) polarimetry and scanning transmission electron microscopy (STEM). SHG polarimetry revealed a variation in the global crystal symmetry of the films from tetragonal (P4mm) to cubic (Pm3¯m) across the composition range, x = 0 to 1 in BaTi1−xSnxO3 (BTSO). STEM imaging shows that the long-range polar order observed when the Sn content is low (x = 0.09) transformed to a short-range polar order as the Sn content increased (x = 0.48). Consistent with atomic displacement measurements from STEM, the largest polarization was obtained at the lowest Sn content of x = 0.09 in Sn-modified BaTiO3 as determined by SHG. These results agree with recent bulk ceramic reports and further identify this material system as a potential replacement for Pb-containing relaxor-based thin film devices.

 

Advances in physical vapor deposition techniques have led to a myriad of quantum materials and technological breakthroughs, affecting all areas of nanoscience and nanotechnology which rely on the innovation in synthesis. Despite this, one area that remains challenging is the synthesis of atomically precise complex metal oxide thin films and heterostructures containing “stubborn” elements that are not only nontrivial to evaporate/sublimate but also hard to oxidize. Here, we report a simple yet atomically controlled synthesis approach that bridges this gap. Using platinum and ruthenium as examples, we show that both the low vapor pressure and the difficulty in oxidizing a “stubborn” element can be addressed by using a solid metal-organic compound with significantly higher vapor pressure and with the added benefits of being in a preoxidized state along with excellent thermal and air stability. We demonstrate the synthesis of high-quality single crystalline, epitaxial Pt, and RuO 2 films, resulting in a record high residual resistivity ratio (=27) in Pt films and low residual resistivity, ∼6 μΩ·cm, in RuO 2 films. We further demonstrate, using SrRuO 3 as an example, the viability of this approach for more complex materials with the same ease and control that has been largely responsible for the success of the molecular beam epitaxy of III-V semiconductors. Our approach is a major step forward in the synthesis science of “stubborn” materials, which have been of significant interest to the materials science and the condensed matter physics community.