Ultrafast Dynamics of Pressure‑Activated Energy Funneling and Amplified Spontaneous Emission in Microscale Quasi-2D Perovskites
Abstract
Abstract Quasi-2D perovskites are attractive for optical gain because of their large exciton binding energies, built-in quantum wells, and efficient energy funneling. However, for micro- and nanolasers, these same properties create a fundamental problem: the energy funnel relies on a statistical mix of different phases, and miniaturize the device inevitably disrupts this delicate distribution—causing the optical gain to collapse. Here we show that high-pressure engineering, a clean and controllable approach, breaks this size-imposed limitation. Applying hydrostatic pressure to microscale (PEA) 2 FA n−1 Pb n Br 3n+1 films rebuilds efficient energy funneling in microscale (PEA) 2 FA n−1 Pb n Br 3n+1 perovskites, activating amplified spontaneous emission (ASE) that is otherwise absent. A modest 0.14 GPa turns on ASE, and at 0.41 GPa the ASE threshold drops by 50%. In situ structural and femtosecond transient absorption measurements reveal a two-step compression-mode transition that directly resolves accelerates energy transfer from low- n to high- n phases and extends the high- n carrier lifetime by 60%. This work uncovers the ultrafast dynamics and photophysical mechanism behind pressure-tuned energy transfer and opens a new route to chip-scale coherent light sources from quasi 2D perovskite film, with direct implications for ultrafast nonlinear optical probes of quantum materials.
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