In recent years, 2D layered organic-inorganic lead halide perovskites have attracted considerable attention due to the distinctive quantum confinement effects as well as prominent excitonic luminescence. Herein, we show that the recombination dynamics and photoluminescence (PL) of the 2D layered perovskites can be tuned by the organic cation length. 2D lead iodide perovskite crystals with increased length of the organic chains reveal blue-shifted PL as well as enhanced relative internal quantum efficiency. Furthermore, we provide experimental evidence that the formation of face-sharing [PbI] octahedron in perovskites with long alkyls induces additional confinement for the excitons, leading to 1D-like recombination. As a result, the PL spectra show enhanced inhomogeneous broadening at low temperature. Our work provides physical understanding of the role of organic cation in the optical properties of 2D layered perovskites, and would benefit the improvement of luminescence efficiency of such materials.

Inorganic−organic hybrid perovskites have drawn considerable attention in photovoltaics and light-emitting diodes (LEDs) due to their exceptional optoelectronic properties. Perovskite multiple quantum wells (MQWs), which employ large organic ammonium cations to form layered structures, have been developed for high-efficiency perovksite LEDs (PeLEDs). However, little is known about the impacts of large organic ammonium cations on the properties of MQW films. In this work, we report MQW perovskites of phenylbutylammonium-cesium lead iodides, which exhibit a photoluminescence peak at 664 nm with a quantum efficiency of 58%. These perovskite MQW films enable red LEDs with high external quantum efficiencies (EQEs) of up to 13.3%. Furthermore, we deposit MQW perovskites of butylammonium-cesium lead iodides. The comparisons of the two perovskite MQW films demonstrate that the choices of large organic ammonium cations significantly influence the properties of the perovskite MQW films, that is, distributions of the quantum-well thicknesses, energy transfer processes, and recombination channels of the emissive centers. Our study shall shed light on the rational design of highperformance perovskite MQW films toward their potential application as red light sources.

All-inorganic lead halide perovskite quantum dots (CsPbBr QDs) are attracting significant research interests because of their highly efficient light-emitting performance combined with tunable emission wavelength facilely realized by ion exchange. However, blue emission from perovskite QDs with strong quantum confinement is rarely reported and suffers from lower luminescence efficiency. Here we report blue-emitting ultrasmall (∼3 nm) CsPbBr QDs with photoluminescence (PL) quantum yield as high as 68%. Using time-resolved and steady-state PL spectroscopy, we elucidate the mechanism of the highly efficient PL as recombination of excitons localized in radiative band tail states. Through analyzing the spectral-dependent PL lifetime and the PL line shape, we obtain a large band tail width of ∼80 meV and a high density of state of ∼10 cm. The relaxation of photocarriers into the radiative tail states suppresses the capture by nonradiative centers. Our results provide solid evidence for the positive role of band tail states in the optical properties of lead halide perovskites, which can be further tailored for high-performance optoelectronic devices.

Solution-processed planar perovskite light-emitting diodes (LEDs) promise high-performance and cost-effective electroluminescent devices ideal for large-area display and lighting applications. Exploiting emission layers with high ratios of horizontal transition dipole moments (TDMs) is expected to boost the photon outcoupling of planar LEDs. However, LEDs based on anisotropic perovskite nanoemitters remain to be inefficient (external quantum efficiency, EQE <5%) due to the difficulties of simultaneously controlling the orientations of TDMs, achieving high photoluminescence quantum yields (PLQYs) and realizing charge balance in the films of assembled nanostructures. Here, we demonstrate efficient electroluminescence from an in situ grown perovskite film composed of a monolayer of face-on oriented nanoplatelets. The ratio of horizontal TDMs of the perovskite nanoplatelet film is ~84%, which leads to a light-outcoupling efficiency of ~31%, substantially higher than that of isotropic emitters (~23%). In consequence, LEDs with a peak EQE of 23.6% are achieved, representing highly efficient planar perovskite LEDs.

Adding alkali metal into lead halide perovskites has recently been demonstrated as an effective strategy for reducing nonradiative loss. However, the suggested role of the alkali metal is usually limited to surface passivation, and the semiconductor doping effect is rarely discussed. Here, the mechanism of lithium doping in the photocarrier recombination in solution‐processed methylammonium lead halide films is investigated by photoluminescence and photoelectron spectroscopies. It is demonstrated that lithium doping weakens the electron–phonon coupling and acts as donor in perovskites, which provide solid evidence that lithium enters the lattice rather than just in the surface region. The n‐type doping creates free electrons to fill the trap states in both the bulk and surface regions, leading to suppressed trapping of photocarriers and reduces nonradiative recombination.