Tartrate‐Assisted Ionic Layer Epitaxy for General Synthesis of 2D Nanostructures

Abstract The synthesis of ultrathin 2D nanomaterials with regular shapes and uniform thickness remains a challenge despite their intriguing properties. In this paper, a facile and generic strategy for the growth of versatile ultrathin nanosheets using tartrate‐assisted ionic layer epitaxy (ILE) at the air‐water interface is presented. Metal ions, stabilized by tartrate coordination, nucleate within the electrical double layer beneath a self‐assembled monolayer. This method facilitates the growth of micro‐sized hexagonal to wafer‐scale continuous nanosheets from 26 metal elements, including single and multi‐element compositions, with high precursor utilization via solution recycling. Furthermore, recognizing the need for efficient quality assessment, the successful application of a multimodal Large Language Model (LLM) for rapid and consistent evaluation of nanosheet quality from microscopy images, achieving performance comparable to human experts is demonstrated. This combined approach demonstrates a sustainable and high‐throughput path for both 2D nanomaterial synthesis and automated quality assessment, accelerating materials discovery.