The inferior crystallinity and phase
stability of CsPbI2Br films have severely hindered the
development of carbon-based,
all-inorganic perovskite solar cells (PSCs). Herein, we demonstrate
the preparation of CsPbI2Br films by the top-seeded solution
growth (TSSG) technique. It is performed through spin-coating of CH3NH3Br (MABr) atop CsPbI2Br precursor
film prior to annealing, during which perovskite seeds are generated
atop it. These perovskite seeds not only serve as nuclei to regulate
the growth of CsPbI2Br grains but also provide additional
Br– anions to generate a thin Br-rich layer atop
the final CsPbI2Br film. The former contributes to the
formation of CsPbI2Br film with full coverage, larger grains,
higher crystallinity, and fewer electronic defects, while the latter
gives rise to residual compressive strain along the film and thus
markedly boosts its phase stability. Consequently, the optimized carbon-based,
all-inorganic PSC exhibits a much better efficiency of 14.84% coupled
with favored storage and operational stability.
All-inorganic, Cl-based
perovskites are promising for visible-blind
UV photodetectors (PDs), particularly the self-powered ones. However,
the devices are rarely reported until now since the low solubility
of raw materials hinders significantly the thickness and electronic
quality of solution-processed Cl-based perovskite films. Herein, we
demonstrate a simple intermediate phase halide exchange method to
prepare desired dual-phase CsPbCl3–Cs4PbCl6 films. It is achieved by spin-coating of a certain
dose of CH3NH3Cl/CsCl solution onto a CsI–PbBr2–dimethyl sulfoxide (DMSO) intermediate phase film,
followed by thermal annealing. The inclusion of CsCl species in the
solution is crucial to a stable dual-phase CsPbCl3–Cs4PbCl6 film, while a high annealing temperature
contributes to improving its quality. Therefore, the dual-phase CsPbCl3–Cs4PbCl6 film with an absorption
onset of ∼420 nm, microsized grains, a few defects, and a proper
work function is obtained by optimizing the annealing temperature.
The final self-powered, visible-blind UV PD exhibits the superior
performance, including a favored response range of 310–420
nm, a high responsivity (R) peak value of 61.8 mA
W–1, an exceptional specific detectivity (D*) maximum of 1.35 × 1012 Jones, and a
particularly fast response speed of 2.1/5.3 μs, together with
amazing operational stability. This work represents the first demonstration
of solution-processed, self-powered, visible-blind UV PDs with all-inorganic,
Cl-based perovskite films.
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