Purcell-Enhanced Spontaneous Emission from Perovskite Quantum Dots Coupled to Plasmonic Crystal

Abstract

Lead halide perovskite quantum dots (PQDs) have recently been proposed as scalable and color-tunable single emitters, but their slow spontaneous emission (1–10 ns) creates a mismatch with high-speed nanophotonic devices. Here, we demonstrate Purcell enhanced emission rate in hybrid structure of PQDs coupled to plasmonic crystal at room temperature. A series of planar devices are produced in large scale via chemistry assembly using colloidal PQDs, Ag nanocubes, and polyvinylpyrrolidone (PVP) as building blocks. By varying the PVP spacer thickness as well as Ag nanocube surface density, a tunable photoluminescence enhancement is realized in both steady and time-resolved measurements. We show a 3.5-fold enhancement in the total fluorescence intensity and simultaneously an increase in the emission rate of a factor of 4.5. Finally, a proof-of-concept tag using PVP spacer encoded inks is demonstrated, providing a promising approach for information security based on Purcell-enhanced emission.

Quantification of the Optical Properties of Perovskite Nanocrystals Using a Combination of Polarized Resonance Synchronous and Polarized Anti-Stokes, On-Resonance, and Stokes-Shifted Spectroscopy

“…Semiconducting lead halide perovskite nanocrystals (PNCs) with a general molecular formula CsPbX 3 (X = Cl, Br, or I) have demonstrated potential in applications including light-emitting devices, solar cells, lasing, and nanophotonics, , owing to their unique optoelectronic characteristics. PNCs exhibit bright and narrow-band photoluminescence (PL) that is tunable from ultraviolet to near-infrared wavelengths by simply changing the halide composition or PNC sizes .…”

Tuning Hybrid exciton–Photon Fano Resonances in Two-Dimensional Organic–Inorganic Perovskite Thin Films

“…With these characteristics, low-dimensional perovskites have emerged as a promising platform for the tailoring of light–matter interactions. Effects like lasing, − enhanced absorption, increased spontaneous emission, − and even Rabi splitting − have been demonstrated, which benefit both conventional optoelectronics, − and may open the path to novel devices like polariton lasers, quantum sensing or optical computation applications. , Controlling distances in these systems is often of great importance, making them attractive targets for biomolecular self-assembly. − Fano resonances are particularly intriguing due to their applications in sensing, switching, and slow light devices. − A Fano resonance − is characterized by asymmetric spectral features and occurs due to the interference of a single, well-defined resonance with a continuum of states or another much broader mode. Originally developed to explain the asymmetric line shapes in the atomic spectra of helium, its theory has been adapted to describe the spectral response in a variety of systems, − including coupling between excitons and plasmonic cavities. − An interesting aspect of LHPs is that due to their high refractive index they can act as optically resonant nanophotonic structures on their own, rendering additional cavities unnecessary.…”

Assembly of Centimeter-Scale Plasmonic Nanocavities for Bright and Ultrafast Emission of Red Carbon Dots

“…Define the emission enhancement factor (EF): EF = I / I 0 , where I and I 0 represent the spectral intensities of coupled (including M and NPA) and uncoupled R-CDs (R), respectively. EF is contributed in three ways: ,, an enhanced excitation efficiency α, an enhancement of light extraction efficiency ζ, and quantum efficiency enhancement (QY/QY 0 ) due to the Purcell effect, i.e., EF = αζQY/QY 0 . The detailed calculation methods and values for three factors (α, ζ, and QY/QY 0 ) could be found in Table S1.…”