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Abstract Excitons in two-dimensional (2D) semiconductors have offered an attractive platform for optoelectronic and valleytronic devices. Further realizations of correlated phases of excitons promise device concepts not possible in the single particle picture. Here we report tunable exciton “spin” orders in WSe₂/WS₂moiré superlattices. We find evidence of an in-plane (xy) order of exciton “spin”—here, valley pseudospin—around exciton fillingv_ex = 1, which strongly suppresses the out-of-plane “spin” polarization. Upon increasingv_exor applying a small magnetic field of ~10 mT, it transitions into an out-of-plane ferromagnetic (FM-z) spin order that spontaneously enhances the “spin” polarization, i.e., the circular helicity of emission light is higher than the excitation. The phase diagram is qualitatively captured by a spin-1/2 Bose–Hubbard model and is distinct from the fermion case. Our study paves the way for engineering exotic phases of matter from correlated spinor bosons, opening the door to a host of unconventional quantum devices. 

Abstract 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 polarization field within the monolayer. While efforts are 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 (V_S andV_Se) and double chalcogen vacancy (V_S−V_Se), interstitial defects (M_i), and metal impurities (M_W) 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.