Narrow Linewidth Spontaneous and Lasing Emissions from Open‐Access Microcavity‐Embedded Perovskite Quantum Dots
Advanced Optical Materials (2025)
Abstract:
Achieving efficient optical coupling between the emission from perovskite quantum dots (PQDs) and photonic integrated elements requires ultranarrow linewidths and highly directional emission. These are challenging goals at room temperature due to the broad and isotropic nature of perovskite emission. Here, we demonstrate ultranarrow‐linewidth emission from CsPbBr3 PQDs at room temperature, in both spontaneous and stimulated regimes, by coupling to state‐of‐the‐art open‐access curved dielectric cavities under continuous wave excitation. The emission is confined to a single transverse electromagnetic mode of the cavity, achieving a remarkably narrow linewidth of 0.2 nm, ≈100× narrower than free‐space emission in both the emission regime. Single‐mode lasing from a small number of PQDs is observed, yielding a quality factor of ≈2590, among the highest reported for single‐mode lasing. The open‐access design enables precise tuning of cavity length and selective coupling of emitters in their native state, overcoming the limitations associated with closed and fixed‐length vertical‐cavity surface emitting laser geometries. The geometry's low divergence and tunability provide an efficient route for integrating perovskite emitters with on‐chip photonic circuits, advancing their use in quantum and optoelectronic technologies. Continuous‐wave lasing from a small number of perovskite quantum dots is achieved by coupling their photoluminescence to open‐access curved dielectric cavities. This geometry confines their emission into a single optical mode, sharply narrowing linewidths in both spontaneous and lasing regimes. Tunable cavity spacing enables precise mode control and high‐Q single‐mode lasing with low divergence emission.Numerical Aperture Dependence of Mie Modes in Low Refractive Index Particles and Enhanced Collection Using Metallic Substrates
Advanced Optical Materials Wiley (2025)
Abstract:
Abstract Advancements in utilizing low refractive index dielectric particles have implications for sensing, lasing, and strong‐coupling at nano and microscopic scales. These cavities offer benefits like ease of fabrication and biocompatibility, making them promising for a wide range of technologies by utilizing their narrow linewidth modes. However, optical modes sustained in these dispersive systems can show distinct behaviors depending on the detection configuration. This study shows the influence of numerical aperture (NA) of the objective lens on the detection of Mie modes in a dielectric microsphere under far‐field excitation and collection. It is demonstrated experimentally and numerically that Mie modes from microspheres outcouple at different angles, with variations in mode amplitudes contingent on the NA of the objective lens, thus leading to distinct linewidths while probing with different NA objectives. Furthermore, it is shown that metallic substrates can facilitate efficient detection of Mie modes by redirecting scattered modes towards low angles. This enables mode detection with low NA lenses and further preventing the inclusion of incident scattered light from higher angles which otherwise perturb the modes. The results underline the importance of careful detection strategies to fully harness dielectric particles as optical platforms for applications in particle detection and characterization.Inhibiting the Appearance of Green Emission in Mixed Lead Halide Perovskite Nanocrystals for Pure Red Emission
Nano Letters American Chemical Society 24:39 (2024) 12045-12053
Abstract:
Mixed halide perovskites exhibit promising optoelectronic properties for next-generation light-emitting diodes due to their tunable emission wavelength that covers the entire visible light spectrum. However, these materials suffer from severe phase segregation under continuous illumination, making long-term stability for pure red emission a significant challenge. In this study, we present a comprehensive analysis of the role of halide oxidation in unbalanced ion migration (I/Br) within CsPbI2Br nanocrystals and thin films. We also introduce a new approach using cyclic olefin copolymer (COC) to encapsulate CsPbI2Br perovskite nanocrystals (PNCs), effectively suppressing ion migration by increasing the corresponding activation energy. Compared with that of unencapsulated samples, we observe a substantial reduction in phase separation under intense illumination in PNCs with a COC coating. Our findings show that COC enhances phase stability by passivating uncoordinated surface defects (Pb2+ and I–), increasing the formation energy of halide vacancies, improving the charge carrier lifetime, and reducing the nonradiative recombination density.Boosting biomolecular switch efficiency with quantum coherence
Physical Review A American Physical Society (APS) 110:1 (2024) 012411
Stability of mixed lead halide perovskite films encapsulated in cyclic olefin copolymer at room and cryogenic temperatures
The Journal of Physical Chemistry Letters American Chemical Society 14:50 (2023) 11333-11341
Abstract:
Lead Mixed Halide Perovskites (LMHPs), CsPbBrI2, have attracted significant interest as promising candidates for wide bandgap absorber layers in tandem solar cells due to their relative stability and red-light emission with a bandgap ∼1.7 eV. However, these materials segregate into Br-rich and I-rich domains upon continuous illumination, affecting their optical properties and compromising the operational stability of devices. Herein, we track the microscopic processes occurring during halide segregation by using combined spectroscopic measurements at room and cryogenic temperatures. We also evaluate a passivation strategy to mitigate the halide migration of Br/I ions in the films by overcoating with cyclic olefin copolymer (COC). Our results explain the correlation between grain size, intensity dependencies, phase segregation, activation energy barrier, and their influence on photoinduced carrier lifetimes. Importantly, COC treatment increases the lifetime charge carriers in mixed halide thin films, improving efficient charge transport in perovskite solar cell applications.