• Taniguchi, Takashi
• Hautier, Geoffroy
• Kudrawiec, Robert
• Gilardoni, Carmem M.
• Watanabe, Kenji
• Atatüre, Mete
• Kopaczek, Jan
• Sayyad, Mohammed
• Yang, Shize
• Chen, Weiru
• Xiong, Yihuang

Abstract

<jats:title>Abstract</jats:title><jats:p>Two‐dimensional (2D) Janus Transition Metal Dichalcogenides (TMDs) have attracted much interest due to their exciting quantum properties arising from their unique two‐faced structure, broken‐mirror symmetry, and consequent colossal polarisation field within the monolayer. While efforts have been made to achieve high‐quality Janus monolayers, the existing methods rely on highly energetic processes that introduce unwanted grain‐boundary and point defects with still unexplored effects on the material's structural and excitonic properties Through High‐resolution scanning transmission electron microscopy (HRSTEM), density functional theory (DFT), and optical spectroscopy measurements; this work introduces the most encountered and energetically stable point defects. It establishes their impact on the material's optical properties. HRSTEM studies show that the most energetically stable point defects are single (<jats:italic>V<jats:sub>S</jats:sub></jats:italic> and <jats:italic>V<jats:sub>Se</jats:sub></jats:italic>) and double chalcogen vacancy (<jats:italic>V<jats:sub>S</jats:sub></jats:italic> −<jats:italic>V<jats:sub>Se</jats:sub></jats:italic>), interstitial defects (M<jats:sub>i</jats:sub>), and metal impurities (M<jats:sub>W</jats:sub>) and establish their structural characteristics. DFT further establishes their formation energies and related localized bands within the forbidden band. Cryogenic excitonic studies on h‐BN‐encapsulated Janus monolayers offer a clear correlation between these structural defects and observed emission features, which closely align with the results of the theory. The overall results introduce the defect genome of Janus TMDs as an essential guideline for assessing their structural quality and device properties.</jats:p><jats:p>This article is protected by copyright. All rights reserved</jats:p>

Topics

• density
• impedance spectroscopy
• grain
• theory
• transmission electron microscopy
• density functional theory
• interstitial
• vacancy
• point defect