Monolayer transition metal dichalcogenides (TMDCs) with high crystalline quality are important channel materials for next‐generation electronics. Researches on TMDCs have been accelerated by the development of chemical vapor deposition (CVD). However, antiparallel domains and twin grain boundaries (GBs) usually form in CVD synthesis due to the special threefold symmetry of TMDCs lattices. The existence of GBs severely reduces the electrical and photoelectrical properties of TMDCs, thus restricting their practical applications. Herein, the epitaxial growth of single crystal MoS2 (SC‐MoS2) monolayer is reported on Au (111) film across a two‐inch c‐plane sapphire wafer by CVD. The MoS2 domains obtained on Au (111) film exhibit unidirectional alignment with zigzag edges parallel to the <110> direction of Au (111). Experimental results indicated that the unidirectional growth of MoS2 domains on Au (111) is a temperature‐guided epitaxial growth mode. The high growth temperature provides enough energy for the rotation of the MoS2 seeds to find the most favorable orientation on Au (111) to achieve a unidirectional ratio of over 99%. Moreover, the unidirectional MoS2 domains seamlessly stitched into single crystal monolayer without GBs formation. The progress achieved in this work will promote the practical applications of TMDCs in microelectronics.

The in-situ polymerization controlled growth of perovskite has been demonstrated as a general strategy to effectively repair grain boundary defects. However, the highly active, volatile, and brittle cross-linked scaffolds of...

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Inorganic cesium lead iodide perovskite CsPbI3 is attracting great attention as a light absorber for single or multi‐junction photovoltaics due to its outstanding thermal stability and proper band gap. However, the device performance of CsPbI3‐based perovskite solar cells (PSCs) is limited by the unsatisfactory crystal quality and thus severe non‐radiative recombination. Here, vacuum‐assisted thermal annealing (VATA) is demonstrated as an effective approach for controlling the morphology and crystallinity of the CsPbI3 perovskite films formed from the precursors of PbI2, CsI, and dimethylammonium iodide (DMAI). By this method, a large‐area and high‐quality CsPbI3 film is obtained, exhibiting a much reduced trap‐state density with prolonged charge lifetime. Consequently, the solar cell efficiency is raised from 17.26 to 20.06 %, along with enhanced stability. The VATA would be an effective approach for fabricating high‐performance thin‐film CsPbI3 perovskite optoelectronics.