Modulating hot carrier relaxation and trapping dynamics in lead halide perovskite nanoplatelets by surface passivation

Abstract

Two-dimensional (2D) lead halide perovskite (LHP) nanoplatelets (NPLs) have recently emerged as promising materials for solar cells and light-emitting devices. The reduction of LHP dimensions introduces an abundance of surface defects, which can strongly influence the photophysical properties of these materials. However, an insightful understanding of the effect of surface defects on hot carrier (HC) relaxation, one of the important properties of LHP NPLs, is still inadequate. Herein, the HC relaxation and trapping dynamics in pristine and surface passivated two-layer (2L) CsPbBr₃ NPLs have been investigated by using time-resolved spectroscopy. The results reveal that surface defects can trap HCs directly before they relax to the band edge, which accounts for the absence of the hot-phonon bottleneck (HPB) effect in LHP NPLs. After healing surface defects with a passivation agent, the relaxation time of HCs is extended from ∼73 to ∼130 fs in 2L CsPbBr₃ NPLs, indicating that the channel of HCs trapped by the surface defects can be effectively blocked. Accordingly, the HPB effect is activated in surface-passivated CsPbBr₃ NPLs. The finding of surface defect-related HC relaxation dynamics is important for guiding the development of high-performance LHP NPL devices related to HCs through surface defect engineering.