Ultrafast Dynamics Across Pressure-Induced Electronic State Transitions, Fluorescence Quenching, and Bandgap Evolution in CsPbBr 3 Quantum Dots.

This work investigates the impact of pressure on the structural, optical properties, and electronic structure of CsPbBr 3 quantum dots (QDs) using steady-state photoluminescence, steady-state absorption, and femtosecond transient absorption spectroscopy, reaching a maximum pressure of 3.38 GPa. The experimental results indicate that CsPbBr 3 QDs undergo electronic state (ES) transitions from ES-I to ES-II and ES-II to ES-III at 0.38 and 1.08 GPa, respectively. Intriguingly, a mixed state of ES-II and ES-III is observed within the pressure range of 1.08-1.68 GPa. The pressure-induced fluorescence quenching in ES-II is attributed to enhanced defect trapping and reduced radiative recombination. Above 1.68 GPa, fluorescence vanishes entirely, attributed to the complete phase transformation from ES-II to ES-III in which radiative recombination becomes non-existent. Notably, owing to stronger quantum confinement effects, CsPbBr 3 QDs exhibit an impressive bandgap tuning range of 0.497 eV from 0 to 2.08 GPa, outperforming nanocrystals by 1.4 times and bulk counterparts by 11.3 times. Furthermore, this work analyzes various carrier dynamics processes in the pressure-induced bandgap evolution and electron state transitions, and systematically studies the microphysical mechanisms of optical properties in CsPbBr 3 QDs under pressure, offering insights for optimizing optical properties and designing novel materials.