Growing clean crystals from dirty precursors: Solid-source metal-organic molecular beam epitaxy growth of superconducting Sr₂RuO₄ films

Ultra-high purity elemental sources have long been considered a prerequisite for obtaining low impurity concentrations in compound semiconductors in the world of molecular beam epitaxy (MBE) since its inception in 1968. However, we demonstrate that a “dirty” solid precursor, ruthenium(III) acetylacetonate [also known as Ru(acac)₃], can yield single-phase, epitaxial, and superconducting Sr₂RuO₄ films with the same ease and control as III-V MBE. A superconducting transition was observed at ∼0.9 K, suggesting a low defect density and a high degree of crystallinity in these films. In contrast to the conventional MBE, which employs the ultra-pure Ru metal evaporated at ∼2000 °C as a Ru source, along with reactive ozone to obtain Ru → Ru⁴⁺ oxidation, the use of the Ru(acac)₃ precursor significantly simplifies the MBE process by lowering the temperature for Ru sublimation (less than 200 °C) and by eliminating the need for ozone. Combining these results with the recent developments in hybrid MBE, we argue that leveraging the precursor chemistry will be necessary to realize next-generation breakthroughs in the synthesis of atomically precise quantum materials.