Robust Ferroelectricity in Nonstoichiometric 2D AgCr_1‐xS₂ via Chemical Vapor Deposition

Abstract Ferroelectricity in two‐dimensional (2D) materials at room temperature has attracted significant interest due to their substantial potential for applications in non‐volatile memory, nanoelectronics, and optoelectronics. The intrinsic tendency of 2D materials toward nonstoichiometry results in atomic configurations that differ from those of their stoichiometric counterparts, thereby giving rise to potential ferroelectric polarization properties. However, reports on the emergence of room temperature ferroelectric effects in nonstoichiometric 2D materials remain limited. This study reports the observation of room temperature ferroelectricity in nonstoichiometric AgCr_1‐xS₂ ternary 2D transition metal dichalcogenides synthesized via chemical vapor deposition. The noncentrosymmetric crystal structure and switchable ferroelectric polarization are confirmed through second harmonic generation (SHG) and piezoresponse force microscopy (PFM) measurements. It is determined that the primary cause of ferroelectric polarization is the interlayer movement of ordered asymmetric Ag atoms under the influence of numerous chromium (Cr) vacancies along with interlayer atom displacement. Furthermore, two types of electrical devices based on in‐plane (IP) and out‐of‐plane (OOP) polarization are demonstrated. This work offers a new perspective for fabricating ternary ultrathin 2D transition metal dichalcogenides ferroelectric materials and presents a potential pathway for creating exceptional multifunctional materials.