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Abstract

Spontaneous formation of charge density wave (CDW) superstructures in monolayers (MLs) of a two-dimensional (2D) crystal lattice is fundamental in understanding its complex quantum states. We report a successful top-down liquid phase exfoliation and stamp transfer process (LPESTP) to create ML VS\textsubscript{2}, undergoing a CDW transition at room temperature. Using high-resolution transmission electron microscopy (HRTEM) and electron diffraction (ED), we observed the coexistence of 1T and 2H polymorphic phases in VS\textsubscript{2} at room temperature, and only the 1T phase undergoes CDW transition. We discovered a novel incommensurate CDW superstructure ($\sqrt{7} \times \sqrt{7}$) R19.1\textsuperscript{o} in ML 1T-VS\textsubscript{2}. With an increase in the number of layers, the CDW order changes to a commensurate ($2 \times 2$) superstructure. Using angle-dependent photoelectron spectroscopy, we have shown that vanadium atoms self-intercalate as V\textsuperscript{3+} ions in multilayer VS\textsubscript{2} and are responsible for the evolution of the CDW superstructure from the incommensurate $\sqrt{7} \times \sqrt{7}$) R 19.1\textsuperscript{o} to the commensurate ($2\times2$) order. We also report the observation of novel Moir\'e superlattices in twisted bilayer 1T-VS\textsubscript{2} flakes with trapped CDW superstructure of the monolayer. Our findings provide an important platform for understanding the evolution of CDW superstructures in 1T-VS\textsubscript{2} with thickness and V self-intercalation.