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An effective passivation technique for AlGaN/GaN high-electron-mobility transistors (HEMTs) is presented. This technique features an AlN thin film grown by plasma-enhanced atomic layer deposition (PEALD). With in situ remote plasma pretreatments prior to the AlN deposition, an atomically sharp interface between ALD-AlN and III-nitride has been obtained. Significant current collapse suppression and dynamic ON-resistance reduction are demonstrated in the ALD-AlN-passivated AlGaN/GaN HEMTs under high-drain-bias switching conditions.