Precise control of the thickness
of large-area two-dimensional
(2D) organometal halide perovskite layers is extremely challenging
owing to the inherent instability of the organic component. Herein,
a novel, highly reproducible, and facile solvothermal route is reported
to synthesize and tailor the thickness and optical band gap of the
organic–inorganic halide perovskite nanosheets (NSs). Our study
reveals that self-assembly of randomly oriented perovskite nanorods
leads to the growth of multilayered perovskite NSs at ∼100
°C, while at higher temperature, large-area few-layer to bilayer
2D NSs (CH3NH3PbBr3) are obtained
through lattice expansion and layer separation depending precisely
on the temperature. Interestingly, the thickness of the 2D NSs shows
a linear dependence on the reaction temperature and thus enables precise
tuning of the thickness from 14 layers to 2 layers, giving rise to
a systematic increase in the band gap and appearance of excitonic
absorption bands. Quantitative analysis of the change in the band
gap with thickness revealed a strong quantum confinement effect in
the 2D layers. The perovskite 2D NSs exhibit tunable color and a high
photoluminescence (PL) quantum yield (QY) up to 84%. Through a careful
analysis of the steady-state and time-resolved PL spectra, the origin
of the lower PL QY in thinner NSs is traced to surface defects in
the 2D layers, for the first time. A white light converter was fabricated
using the composition-tuned 2D CH3NH3PbBrI2 NS on a blue light-emitting diode chip. The 2D perovskite
photodetector exhibits a stable and very fast rise/fall time (24 μs/103
μs) along with high responsivity and detectivity of ∼1.93
A/W and 1.04 × 1012 Jones, respectively. Storage,
operational, and temperature-dependent stability studies reveal high
stability of the 2D perovskite NSs under the ambient condition with
high humidity. The reported method is highly promising for the development
of large-area stable 2D perovskite layers for various cutting-edge
optoelectronic applications.