To
resolve the inherent trade-off issue between responsivity and detectivity
in FA0.9Cs0.1PbI3 perovskite photodetectors,
this paper proposes a novel strategy using multifunctional self-combustion
additives (urea and ammonium nitrate). During the early stages of
crystallization, urea allows for the formation of a strong Lewis complex-derived
low-dimensional intermediate phase; this suppresses the formation
of perovskite nuclei, while ammonium ions assist the preferred grain
growth along the [110] direction. During the high-temperature annealing
steps, a self-combusting exothermic reaction occurs between urea as
a fuel and NH4NO3 as an oxidizer, through which
a locally supplied heat facilitates the removal of residual urea and
byproducts. These multifunctional roles of self-combustible additives
facilitate the production of high-quality, enlarged grain-structured
perovskite films with improved optoelectronic properties, as confirmed
by various analyses, including impedance spectroscopy and intensity-modulated
photocurrent spectroscopy. The resulting FA0.9Cs0.1PbI3-based photodiode-type photodetectors exhibit outstanding
performance, such as a high responsivity (0.762 A W–1) and specific detectivity (over 5.08 × 1013 Jones)
at a very low external reverse bias (−0.5 V). Our findings
clearly suggest that the multifunctional self-combustion additives
strategy could help realize the full potential of FA1–x
Cs
x
PbI3 as
a photodiode-type photodetector.