Colloidal metal-halide perovskite quantum dots (QDs) with a dimension less than the exciton Bohr diameter D (quantum size regime) emerged as promising light emitters due to their spectrally narrow light, facile color tuning, and high photoluminescence quantum efficiency (PLQE). However, their size-sensitive emission wavelength and color purity and low electroluminescence efficiency are still challenging aspects. Here, we demonstrate highly efficient light-emitting diodes (LEDs) based on the colloidal perovskite nanocrystals (NCs) in a dimension > D (regime beyond quantum size) by using a multifunctional buffer hole injection layer (Buf-HIL). The perovskite NCs with a dimension greater than D show a size-irrespective high color purity and PLQE by managing the recombination of excitons occurring at surface traps and inside the NCs. The Buf-HIL composed of poly(3,4-ethylenedioxythiophene)/poly(styrenesulfonate) (PEDOT:PSS) and perfluorinated ionomer induces uniform perovskite particle films with complete film coverage and prevents exciton quenching at the PEDOT:PSS/perovskite particle film interface. With these strategies, we achieved a very high PLQE (∼60.5%) in compact perovskite particle films without any complex post-treatments and multilayers and a high current efficiency of 15.5 cd/A in the LEDs of colloidal perovskite NCs, even in a simplified structure, which is the highest efficiency to date in green LEDs that use colloidal organic-inorganic metal-halide perovskite nanoparticles including perovskite QDs and NCs. These results can help to guide development of various light-emitting optoelectronic applications based on perovskite NCs.

Size-controlled graphene quantum dots (GQDs) are prepared via amidative cutting of tattered graphite. The power of this method is that the size of the GQDs could be varied from 2 to over 10 nm by simply regulating the amine concentration. The energy gaps in such GQDs are narrowed down with increasing their size, showing colorful photoluminescence from blue to brown. We also reveal the roles of defect sites in photoluminescence, developing long-wavelength emission and reducing exciton lifetime. To assess the viability of the present method, organic light-emitting diodes employing our GQDs as a dopant are first demonstrated with the thorough studies in their energy levels. This is to our best knowledge the first meaningful report on the electroluminescence of GQDs, successfully rendering white light with the external quantum efficiency of ca. 0.1%.

Carbon nanodots (C-dots) are a kind of fluorescent carbon nanomaterials, composed of polyaromatic carbon domains surrounded by amorphous carbon frames, and have attracted a great deal of attention because of their interesting properties. There are still, however, challenges ahead such as blue-biased photoluminescence, spectral broadness, undefined energy gaps and etc. In this report, we chemically modify the surface of C-dots with a series of para-substituted anilines to control their photoluminescence. Our surface functionalization endows our C-dots with new energy levels, exhibiting long-wavelength (up to 650 nm) photoluminescence of very narrow spectral widths. The roles of para-substituted anilines and their substituents in developing such energy levels are thoroughly studied by using transient absorption spectroscopy. We finally demonstrate light-emitting devices exploiting our C-dots as a phosphor, converting UV light to a variety of colors with internal quantum yields of ca. 20%.

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Chemically derived graphene quantum dots (GQDs) to date have showed very broad emission linewidth due to many kinds of chemical bondings with different energy levels, which significantly degrades the color purity and color tunability. Here, we show that use of aniline derivatives to chemically functionalize GQDs generates new extrinsic energy levels that lead to photoluminescence of very narrow linewidths. We use transient absorption and time-resolved photoluminescence spectroscopies to study the electronic structures and related electronic transitions of our GQDs, which reveals that their underlying carrier dynamics is strongly related to the chemical properties of aniline derivatives. Using these functionalized GQDs as lumophores, we fabricate light-emitting didoes (LEDs) that exhibit green, orange, and red electroluminescence that has high color purity. The maximum current efficiency of 3.47 cd A−1 and external quantum efficiency of 1.28% are recorded with our LEDs; these are the highest values ever reported for LEDs based on carbon-nanoparticle phosphors. This functionalization of GQDs with aniline derivatives represents a new method to fabricate LEDs that produce natural color.