Solution-Based Synthesis of Layered Two-Dimensional Oxides as Broadband Emitters.

Abstract

Preparing transition-metal oxides in their two-dimensional (2D) form is the key to exploring their unrevealed low-dimensional properties, such as the p<i>-</i>type transparent superconductivity, topological Mott insulator state, existence of the condensed 2D electron/hole gas, and strain-tunable catalysis. However, existing approaches suffer from the specific constraint techniques and precursors that limit their product types. Here, we report a solution-based method to directly synthesize KNbO₂ in 2D by an out-of-the-pot growth process at low temperature, which is observed directly in real time. The developed method can also be applied to other 2D ternary oxide syntheses, including CsNbO₂ and composited Na_<i>x</i>K_1-<i>x</i>NbO₂, and it can be extended to the preparation of self-assembled nanofilms. In addition, We demonstrate the emission of broadband photoluminescence (PL, λ ∼ 350-800 nm) from as-synthesized single-crystal 2D KNbO₂ sheets down to a single unit cell thickness. The ultra-broadband emission is ascribed to the self-trapped excitation state (STEs) from the in-phase distortion of the NbO₆ octahedrons in 2D NbO₂^- layers. Beyond the broader luminescent range and the robust material thermal stability of niobates, the absence of sample size restrictions and the large aspect ratio of the 2D oxide sheets will provide opportunities in miniaturizing and advancing 2D-materials integrated optoelectronic devices.