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The recent synthesis of monolayer MoSi2N4, along with theoretical predictions encompassing the entire family of its chemical analogs, has opened up a new array of low‐dimensional materials for a diverse range of optoelectronics and photovoltaics applications. In this first‐principles many‐body study, the quasiparticle electronic structure of the material class MSi2Z4 (M = Mo, W, and Z = N, P, As,...