Electroluminescence efficiencies and stabilities of quasi-two-dimensional halide perovskites are restricted by the formation of multiple-quantum-well structures with broad and uncontrollable phase distributions. Here, we report a ligand design strategy to substantially suppress diffusion-limited phase disproportionation, thereby enabling better phase control. We demonstrate that extending the π-conjugation length and increasing the cross-sectional area of the ligand enables perovskite thin films with dramatically suppressed ion transport, narrowed phase distributions, reduced defect densities, and enhanced radiative recombination efficiencies. Consequently, we achieved efficient and stable deep-red light-emitting diodes with a peak external quantum efficiency of 26.3% (average 22.9% among 70 devices and cross-checked) and a half-life of ~220 and 2.8 h under a constant current density of 0.1 and 12 mA/cm2, respectively. Our devices also exhibit wide wavelength tunability and improved spectral and phase stability compared with existing perovskite light-emitting diodes. These discoveries provide critical insights into the molecular design and crystallization kinetics of low-dimensional perovskite semiconductors for light-emitting devices.

Quantum emitters coupled to plasmonic nanostructures can act as exceptionally bright sources of single photons, operating at room temperature. Plasmonic mode volumes supported by these nanostructures can be several orders of magnitude smaller than the cubic wavelength, which leads to dramatically enhanced light-matter interactions and drastically increased photon production rates. However, when increasing the light localization further, these deeply subwavelength modes may in turn hinder the fast outcoupling of photons into free space. Plasmonic hybrid nanostructures combining a highly confined cavity mode and a larger antenna mode circumvent this issue. We establish the fundamental limits for quantum emission enhancement in such systems and find that the best performance is achieved when the cavity and antenna modes differ significantly in size. We experimentally support this idea by photomodifying a nanopatch antenna deterministically assembled around a nanodiamond known to contain a single nitrogen-vacancy (NV) center. As a result, the cavity mode shrinks, further shortening the NV fluorescence lifetime and increasing the single-photon brightness. Our analytical and numerical simulation results provide intuitive insight into the operation of these emitter-cavity-antenna systems and show that this approach could lead to single-photon sources with emission rates up to hundreds of THz and efficiencies close to unity.

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Transparent conducting oxides, such as doped indium oxide, zinc oxide, and cadmium oxide (CdO), have recently attracted attention as tailorable materials for applications in nanophotonic and plasmonic devices such as low‐loss modulators and all‐optical switches due to their tunable optical properties, fast optical response, and low losses. In this work, optically induced extraordinarily large reflection changes (up to 135%) are demonstrated in bulk CdO films in the mid‐infrared wavelength range close to the epsilon near zero (ENZ) point. To develop a better understanding of how doping level affects the static and dynamic optical properties of CdO, the evolution of the optical properties with yttrium (Y) doping is investigated. An increase in the metallicity and a blueshift of the ENZ point with increasing Y‐concentrations is observed. Broadband all‐optical switching from near‐infrared to mid‐infrared wavelengths is demonstrated. The major photoexcited carrier relaxation mechanisms in CdO are identified and it is shown that the relaxation times can be significantly reduced by increasing the dopant concentration in the film. This work could pave the way to practical dynamic and passive optical and plasmonic devices with doped CdO spanning wavelengths from the ultraviolet to the mid‐infrared region.

Plasmonic color printing with semicontinuous metal films is a lithography-free and environment-friendly method for generating non-fading bright colors. Such films are comprised of islands -metal nanoparticles and their clusters of various dimensions, which resonate at different wavelengths upon external light illumination depending on the size and 2 shape of the local particle structures. To experimentally realize systems that were optimized for achieving a broad color range and increased stability, various silver semicontinuous metal films were deposited on a metallic (Ag) mirror with a sub-wavelength-thick dielectric (SiO2) spacer. Femtosecond laser post-processing was then introduced to extend the color gamut through spectrally induced changes from blue to green, red, and yellow. Long-term stability and durability of the structures were addressed to enable non-fading colors with an optimized overcoating dielectric layer. The thickness of the proposed design is on the order of 100 nanometers, and it can be deposited on any substrate. These structures generate a broad range of long-lasting colors in reflection that can be applied to real-life artistic or technological applications with a spatial resolution on the order of 0.3 mm or less.