Bottom surface of active layers and interface of indium tin oxide (ITO) electrodes and active layers play a crucial role in determining the performance of polymer photodetectors with photomultiplication (PM-PPDs). The interfacial trapped electron distribution closing to ITO electrodes will determine spectral response range and external quantum efficiency (EQE) of PM-PPDs. The bottom interface is more sensitive than top interface when light is coming from the ITO side, and the larger density of generated charge on the bottom interfaces will induce interfacial band more bending for efficient charge tunneling injection. Highly sensitive and sub-microsecond PM-PPDs are achieved with PMBBDT:Y6 (100:7, w/w) as active layers under forward bias, yielding EQE of 18,700% at 320 nm, 21,700% at 600 nm and 16,400% at 810 nm under a bias of 7 V, respectively, as well as fast response time of 79 μs. The high EQE of the PM-PPDs is attributed to efficient hole tunneling injection from ITO electrode under forward bias. The electron traps closing to ITO electrode will be quickly filled up when light is coming from ITO side, leading to interfacial band more bending for hole tunneling injection. Importantly, the PM-PPDs is performed to measure heart rate (HR) and blood oxygen saturation (SpO 2 ), and the measured data by the PM-PPDs are very similar with those obtained by commercial photodetectors.

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