Organometallic
halide perovskites are a class of solution-processed
semiconductors exhibiting remarkable optoelectronic properties. They
have seen rapid strides toward enabling efficient third-generation
solar cell technologies. Here, we report the first material-tailoring
of TiO2/perovskite/spiro-OMeTAD junction-based photodiodes
toward applications in photodetection, a field in need of fast, sensitive,
low-cost, spectrally tunable materials that offer facile integration
across a broad range of substrates. We report photodetection that
exhibits 1 μs temporal response, and we showcase stable operation
in the detection of over 7 billion transient light pulses through
a continuous pulsed-illumination period. The perovskite diode photodetector
has a peak responsivity approaching 0.4 A W–1 at
600 nm wavelength, which is superior to red light detection in crystalline
silicon photodiodes used in commercial image sensors. Only by developing
a composite Al2O3/PCBM front contact interface
layer were we able to stabilize device operation in air, reduce dark
current, and enhance the responsivity in the low-bias regime to achieve
an experimentally measured specific detectivity of 1012 Jones.