Effects of Pressure on Exciton Absorption and Emission in Strongly Quantum-Confined CsPbBr3 Quantum Dots and Nanoplatelets.

Abstract

Soft lattices of metal halide perovskite (MHP) nanocrystals (NCs) are considered responsible for many of their optical properties associated with excitons, which are often distinct from other semiconductor NCs. Earlier studies of MHP NCs upon compression revealed how structural changes and the resulting changes in the optical properties such as the bandgap can be induced at relatively low pressures. However, the pressure response of the exciton transition itself in MHP NCs remains relatively poorly understood due to limitations inherent to studying weakly or nonconfined NCs in which exciton absorption peaks are not well-separated from the continuum interband transition. Here, we investigated the pressure response of the absorbing and emitting transitions of excitons using strongly quantum-confined CsPbBr3 quantum dots (QDs) and nanoplatelets (NPLs), which both exhibit well-defined exciton absorption peaks. Notably, the reversible vanishing and recovery of the exciton absorption accompanied by reversible quenching and recovery of the emission were observed in both QDs and NPLs, resulting from the reversible pressure modulation of the exciton oscillator strength. Furthermore, CsPbBr3 NPLs exhibited irreversible pressure-induced creation of trap states at low pressures (∼0.1 GPa) responsible for trapped exciton emission that developed on the time scale of ∼10 min, while the reversible pressure response of the absorbing exciton transition was maintained. These findings shed light on the diverse effects the application of force has on the absorbing and emitting exciton transitions in MHP NCs, which are important for their application as excitonic light emitters in high-pressure environments.