Superfluorescence is a quantum optical phenomenon in which an initially excited ensemble of incoherent dipoles first acquire macroscopic coherence and then collectively recombine and radiate a burst of photons. This process is a symmetry breaking macroscopic quantum phase transition similar to superconductivity and Bose-Einstein condensation. Since quantum coherence is extremely fragile at high temperatures, similar to other macroscopic quantum phase transitions, superfluorescence has been almost always observed at cryogenic temperatures. In this presentation I will first present our results on room temperature superfluorescence in lead-halide perovskites and then present the mechanism that enables this exotic quantum phase transition at room temperature.
In this work, we demonstrated that through the addition of large organic cation PEABr, the quality of cesium lead halide thin films has been enhanced by controlling the crystallization process and thus the domain size and morphology. As a result, by increasing the PEABr concentration to 40%, the perovskite thin films with a small domain size, highly oriented crystal structure and low defect density demonstrated a lowest amplified spontaneous emission threshold of 7 µJ/cm2. However, further increasing PEABr concentration will result in a slower energy transfer, which limits the population inversion process and thus showed a higher ASE threshold. Using this strategy, by tuning the halide ratio, the ASE emissions were observed over the broad visible range (from 490 nm to 680 nm), demonstrating its wide wavelength-tunability.
Quasi-2D Ruddlesden-Popper halide perovskites with a large exciton binding energy, self-assembled quantum wells and high quantum yield draw attention for optoelectronic device applications. Thin films of these quasi-2D perovskites consist of a mixture of domains having different dimensionality, allowing energy funneling from lower-dimensional nanosheets (narrower bandgap domains) to three-dimensional nanocrystals (wide bandgap domains). Here, the quality of quasi-2D perovskite (PEA)2(FA)3Pb4Br13 is controlled by solution engineering. Grazing-incidence wide-angle X-ray scattering (GIWAXS) measurements were conducted to study the crystal orientation, and transient absorption spectroscopy (TAS) measurements were conducted to study the charge carrier dynamics. Our data show that the highly oriented 2D crystals have a faster energy transfer to the low bandgap regime (< 0.5 ps) compared to less oriented films. High-performance LEDs can be realized with these 2D films. Finally, amplified spontaneous emission is achieved with an ultralow threshold of 4.16 μJ/cm2 and distributed feedback lasers are realized.
Our results show that it is important to control the morphology and spatial domain distribution of the quasi-2D films to achieve efficient energy transfer, which is a critical requirement for optoelectronic devices.
Access to the requested content is limited to institutions that have purchased or subscribe to SPIE eBooks.
You are receiving this notice because your organization may not have SPIE eBooks access.*
*Shibboleth/Open Athens users─please
sign in
to access your institution's subscriptions.
To obtain this item, you may purchase the complete book in print or electronic format on
SPIE.org.
INSTITUTIONAL Select your institution to access the SPIE Digital Library.
PERSONAL Sign in with your SPIE account to access your personal subscriptions or to use specific features such as save to my library, sign up for alerts, save searches, etc.