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2D metal oxides (2DMOs) have recently emerged as a high‐performance class of ultrathin, wide bandgap materials offering exceptional electrical and optical properties for a wide area of device applications in energy, sensing, and display technologies. Liquid metal printing represents a thermodynamically advantageous strategy for synthesizing 2DMOs by a solvent‐free and vacuum‐free scalable method. Here, recent progress in the field of liquid metal printed 2D oxides is reviewed, considering how the physics of Cabrera‐Mott oxidation gives this rapid, low‐temperature process advantages over alternatives such as sol‐gel and nanoparticle processing. The growth, composition, and crystallinity of a burgeoning set of 1–3 nm thick liquid metal printed semiconducting, conducting, and dielectric oxides are analyzed that are uniquely suited for the fabrication of high‐performance flexible electronics. The advantages and limitations of these strategies are considered, highlighting opportunities to amplify the impact of 2DMO through large‐area printing, the design of doped metal alloys, stacking of 2DMO to electrostatically engineer new oxide heterostructures, and implementation of 2D oxide devices for gas sensing, photodetection, and neuromorphic computing.

 

2D native surface oxides formed on low melting temperature metals such as indium and gallium offer unique opportunities for fabricating high-performance flexible electronics and optoelectronics based on a new class of liquid metal printing (LMP). An inherent property of these Cabrera-Mott 2D oxides is their suboxide nature (e.g., In2O3−x), which leads high mobility LMP semiconductors to exhibit high electron concentrations (ne > 1019 cm−3) limiting electrostatic control. Binary alloying of the molten precursor can produce doped, ternary metal oxides such as In-X-O with enhanced electronic performance and greater bias-stress stability, though this approach demands a deeper understanding of the native oxides of alloys. This work presents an approach for hypoeutectic rapid LMP of crystalline InGaOx (IGO) at ultralow process temperatures (180 °C) beyond the state of the art to fabricate transistors with 10X steeper subthreshold slope and high mobility (≈18 cm2 Vs−1). Detailed characterization of IGO crystallinity, composition, and morphology, as well as measurements of its electronic density of states (DOS), show the impact of Ga-doping and reveal the limits of doping induced amorphization from hypoeutectic precursors. The ultralow process temperatures and compatibility with high-k Al2O3 dielectrics shown here indicate potential for 2D IGO to drive low-power flexible transparent electronics. 

We present a rapid liquid metal printing process (CLMP) enabling fabrication of high-mobility metal oxide semiconducting channels in less than 3 seconds. We use this process to engineer heterostructure TFTs with channels consisting of 3 nm layers of In2O3 and Ga2O3 with improved subthreshold slope and enhanced on-state performance (uave∼14cm2/Vs) . We report the influence of deposition temperature and speed, investigating crystallinity and grain morphology of this class of 2D oxide semiconductors.