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The high defect density on the surface of AlGaN material with high Al composition limits its application in the field of solar-blind ultraviolet (UV) detection. In this work, a surface modification method for AlGaN has been proposed to enhance the performance of AlGaN metal-semiconductor-metal (MSM) solar-blind UV photodetectors (PDs). The 5,10,15,20-T(4-OH P)P (C 44 H 30 N 4 O 4 ) organic molecules are chemically adsorbed on the surface of high-Al-content Al 0.6 Ga 0.4 N MSM PD, which can reduce the interface potential caused by material defects and increase the photogenerated carriers of the device. Compared with the control unmodified PD, the C 44 H 30 N 4 O 4 modification method significantly increases the photocurrent and responsivity of the PD, which is beneficial to improve the optoelectronic performances of III-nitride-based PDs.