AbstractCoupling together the ferroelectric, pyroelectric, and photovoltaic characteristics within a single material is a novel way to improve the performance of photodetectors. In this work, we take advantage of the triple multifunctionality shown by 0.5Ba(Zr0.2Ti0.8)O3–0.5(Ba0.7Ca0.3)TiO3 (BCZT), as demonstrated in an Al/Si/SiOx/BCZT/ITO thin‐film device. The Si/SiOx acts as an n‐type layer to form a metal–ferroelectric–insulator–semiconductor heterostructure with the BCZT, and with Al and ITO as electrodes. The photo‐response of the device, with excitation from a violet laser (405 nm wavelength), is carefully investigated, and it is shown that the photodetector performance is invariant with the chopper frequency owing to the pyro‐phototronic effect, which corresponds to the coupling together of the pyroelectric and photovoltaic responses. However, the photodetector performance was significantly better than that of the devices operating based only on the pyro‐phototronic effect by a factor of 4, due to the presence of ferroelectricity in the system. Thus, after a poling voltage of −15 V, for a laser power density of 230 mW/cm2 and at a chopper frequency of 400 Hz, optimized responsivity, detectivity, and sensitivity values of 13.1 mA/W, 1.7 × 1010 Jones, and 26.9, respectively, are achieved. Furthermore, ultrafast rise and fall times of 2.4 and 1.5 µs, respectively, are obtained, which are 35,000 and 36,000 times faster rise and fall responses, respectively, than previous reports of devices with the ferro–pyro–phototronic effect. This is understood based on the much faster ferroelectric switching in ferroelectric thin films owing to the predominant 180° domains in a single direction out of plane.
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