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Chlorination surface treatment was used to improve the performance of GaN-based ultraviolet metal–semiconductor–metal photodetectors (MSM-PDs). The noise equivalent power of chlorine-treated MSM-PDs measured at 5 V was 1.60 × 10-12 W, which was less than that of untreated ones (6.68 × 10-12 W). The normalized detectivity of chlorine-treated MSM-PDs was 1.90 × 1011 cm Hz0.5 W-1, which was higher than the measured value of 4.72 × 1010 cm Hz0.5 w-1 of untreated ones. The dark current of chlorine-treated and untreated MSM-PDs operating at 10 V was 21.4 and 762.0 pA, respectively. The improvement was attributed to the passivation of the GaN surface and the reduction of surface states as a result of the chlorination surface treatment.