KCl acts as a flux to assist the growth of sub-millimeter-scale metallic 2D non-layered molybdenum dioxide

Two-dimensional (2D) metal oxides (2DMOs), such as MoO2, have made impressive strides in recent years, and their applicability in a number of fields such as electronic devices, optoelectronic devices and lasers has been demonstrated. However, 2DMOs present challenges in their synthesis using conventional methods due to their non-van der Waals nature. We report that KCl acts as a flux to prepare large-area 2DMOs with sub-millimeter scale. We systematically investigate the effects of temperature, homogeneous time and cooling rate on the products in the flux method, demonstrating that in this reaction a saturated homogenous solution is obtained upon the melting of the salt and precursor. Afterward, the cooling rate was adjusted to regulate the thickness of the target crystals, leading to the precipitation of 2D non-layered material from the supersaturated solution; by applying this method, the highly crystalline non-layered 2D MoO2 flakes with so far the largest lateral size of up to sub-millimeter scale (similar to 464 mu m) were yielded. Electrical studies have revealed that the 2D MoO2 features metallic properties, with an excellent sheet resistance as low as 99 Omega center dot square(-1) at room temperature, and exhibits a property of charge density wave in the measurement of resistivity as a function of temperature.