The ferro-pyro-phototronic (FPP) effect, coupling photoexcited pyroelectricity and photovoltaics, paves an effective way to modulate charge-carrier behavior of optoelectronic devices. However, reports of promising FPP-active systems remain quite scarce due to a lack of knowledge on the coupling mechanism. Here, we have successfully enhanced the FPP effect in a series of ferroelectrics, BACsMAPbBr (BA = butylammonium, MA = methylammonium, 0 ≤ ≤ 0.34), rationally assembled by mixing cage cations into 2D metal-halide perovskites. Strikingly, chemical alloying of Cs/MA cations leads to the reduction of exciton binding energy, as verified by the = 0.34 component; this facilitates exciton dissociation into free charge-carriers and boosts photo-activities. The crystal detector thus displays enhanced FPP current at zero bias, almost more than 10 times higher than that of the = 0 prototype. As an innovative study on the FPP effect, this work affords new insight into the fundamental principle of ferroelectrics and creates a new strategy for self-driven photodetection.

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http://www.ncbi.nlm.nih.gov/pmc/articles/PMC10530782PMC
http://dx.doi.org/10.1039/d3sc02946hDOI Listing

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