Light‐Triggered Reversible Assembly of Halide Perovskite Nanoplatelets

Abstract Advancements in stimuli‐driven nanoactuators necessitate the discovery of photo‐switchable, self‐contained semiconductor nanostructures capable of precise mechanical responses. The reversible assembly of 0D Cs 3 Bi 2 I 9 halide perovskite nanoplatelets (NPLs) between stacked and scattered configurations are demonstrated under light and dark, respectively. This sunlight‐triggered perpetual flipping of the NPLs, occurring in less than a minute, is associated with a color change between brown and red. The photomechanical response is driven by the formation and cleavage of sulfide linkages at the NPL surface. In the stacked configuration, various stacking modes create moiré superstructures, enhancing the interlayer charge distribution, and increasing the electronic conductivity and optical absorbance. This leads to a decrease in exciton binding energy from 247 meV for scattered NPLs to 162 meV for stacked NPLs, resulting in a 3.5‐fold enhancement in dark current for the stacked NPL films. The switchable control over color and electric current is continuously reversible and retraceable, exhibiting a minor memory effect observed during extended cycling. The self‐flipping NPL nanoactuators demonstrate reversible mechanical responses, with topographical oscillations ranging from 14 nm in scattered NPLs to 50 nm in the vertically stacked configuration. This seamless reversible nano‐assembly with color interchangeability offers numerous possibilities for nanorobotics, nanoscale switches, and sensors.