Controllable and Fast Growth of High-Quality Atomically Thin and Atomically Flat Bi$_2$O$_2$Se Films

As a novel and promising 2D material, bismuth oxyselenide (Bi$_2$O$_2$Se) has demonstrated significant potential to overcome existing technical barriers in various electronic device applications, due to its unique physical properties like high symmetry, adjustable electronic structure, ultra-high electron mobility. However, the rapid growth of Bi$_2$O$_2$Se films down to a few atomic layers with precise control remains a significant challenge. In this work, the growth of two-dimensional (2D) Bi$_2$O$_2$Se thin films by the pulsed laser deposition (PLD) method is systematically investigated. By controlling temperature, oxygen pressure, laser energy density and laser emission frequency, we successfully prepare atomically thin and flat Bi$_2$O$_2$Se (001) thin films on the (001) surface of SrTiO3. Importantly, we provide a fundamental and unique perspective toward understanding the growth process of atomically thin and flat Bi$_2$O$_2$Se films, and the growth process can be primarily summarized into four steps: i) anisotropic non-spontaneous nucleation preferentially along the step roots; ii) monolayer Bi$_2$O$_2$Se nanosheets expanding across the surrounding area, and eventually covering the entire STO substrate step; iii) vertical growth of Bi$_2$O$_2$Se monolayer in a 2D Frank-van der Merwe (FM) epitaxial growth, and iv) with a layer-by-layer 2D FM growth mode, ultimately producing an atomically flat and epitaxially aligned thin film. Moreover, the combined results of the crystallinity quality, surface morphology and the chemical states manifest the successful PLD-growth of high-quality Bi$_2$O$_2$Se films in a controllable and fast mode.