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GaN films are prepared via double‐polarity selective‐area growth (DP‐SAG) using metal‐organic vapor‐phase epitaxy. Here, we demonstrate an improved DP‐SAG process using a carbon mask and an initial Ga‐polar GaN layer to fabricate a GaN film consisting of periodic Ga‐polar and N‐polar domains. The GaN films with periodically poled structures (alternating Ga‐polar and N‐polar regions) can serve as...