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Principles Of Fluorescence Spectroscopy

The visualization of accurate colour information using quantum dots has been explored for decades, and commercial products employing environmentally friendly materials are currently available as backlights1. However, next-generation electroluminescent displays based on quantum dots require the development of an efficient and stable cadmium-free blue-light-emitting device, which has remained a challenge because of the inferior photophysical properties of blue-light-emitting materials2,3. Here we present the synthesis of ZnSe-based blue-light-emitting quantum dots with a quantum yield of unity. We found that hydrofluoric acid and zinc chloride additives are effective at enhancing luminescence efficiency by eliminating stacking faults in the ZnSe crystalline structure. In addition, chloride passivation through liquid or solid ligand exchange leads to slow radiative recombination, high thermal stability and efficient charge-transport properties. We constructed double quantum dot emitting layers with gradient chloride content in a light-emitting diode to facilitate hole transport, and the resulting device showed an efficiency at the theoretical limit, high brightness and long operational lifetime. We anticipate that our efficient and stable blue quantum dot light-emitting devices can facilitate the development of electroluminescent full-colour displays using quantum dots. Cadmium-free blue quantum dot light-emitting diodes are constructed with a quantum yield of unity, an efficiency at the theoretical limit, high brightness and long operational lifetime.

Efficient and stable blue quantum dot light-emitting diode.

Colloidal nanocrystals are nanometer-sized, solution-grown inorganic particles stabilized by a layer of surfactants attached to their surface. The inorganic cores exhibit useful properties controlled by composition as well as size and shape, while the surfactant coating ensures that these structures are easy to fabricate and process. It is this combination of features that makes colloidal nanocrystals attractive and promising building blocks for advanced materials and devices. But their full potential can only be exploited if we achieve exquisite control over their composition, size, shape, crystal structure and surface properties. Here we review what is known about nanocrystal growth and outline strategies for controlling it.

Colloidal nanocrystal synthesis and the organic-inorganic interface

Colloidal quantum dots are promising emitters for quantum-dot-based light-emitting-diodes. Though quantum dots have been synthesized with efficient, stable, and high colour-purity photoluminescence, inheriting their superior luminescent properties in light-emitting-diodes remains challenging. This is commonly attributed to unbalanced charge injection and/or interfacial exciton quenching in the devices. Here, a general but previously overlooked degradation channel in light-emitting-diodes, i.e., operando electrochemical reactions of surface ligands with injected charge carriers, is identified. We develop a strategy of applying electrochemically-inert ligands to quantum dots with excellent luminescent properties to bridge their photoluminescence-electroluminescence gap. This material-design principle is general for boosting electroluminescence efficiency and lifetime of the light-emitting-diodes, resulting in record-long operational lifetimes for both red-emitting light-emitting-diodes (T95 > 3800 h at 1000 cd m−2) and blue-emitting light-emitting-diodes (T50 > 10,000 h at 100 cd m−2). Our study provides a critical guideline for the quantum dots to be used in optoelectronic and electronic devices. New design principles for bridging the photoluminescence and electroluminescence of colloidal quantum dots are needed. In this work, the authors report electrochemically-inert ligands as a general material-design strategy for realizing high-performance LEDs based on quantum dots.

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Electrochemically-stable ligands bridge the photoluminescence-electroluminescence gap of quantum dots.

The research on metal halide perovskite light-emitting diodes (PeLEDs) with green and infrared emission has demonstrated significant progress in achieving higher functional performance. However, the realization of stable pure-blue (≈470 nm wavelength) PeLEDs with increased brightness and efficiency still constitutes a considerable challenge. Here, a novel acid etching-driven ligand exchange strategy is devised for achieving pure-blue emitting small-sized (≈4 nm) CsPbBr3 perovskite quantum dots (QDs) with ultralow trap density and excellent stability. The acid, hydrogen bromide (HBr), is employed to etch imperfect [PbBr6 ]4- octahedrons, thereby removing surface defects and excessive carboxylate ligands. Subsequently, didodecylamine and phenethylamine are successively introduced to bond the residual uncoordinated sites of the QDs and attain in situ exchange with the original long-chain organic ligands, resulting in near-unity quantum yield (97%) and remarkable stability. The QD-based PeLEDs exhibit pure-blue electroluminescence at 470 nm (corresponding to the Commission Internationale del'Eclairage (CIE) (0.13, 0.11) coordinates), an external quantum efficiency of 4.7%, and a remarkable luminance of 3850 cd m-2 , which is the highest brightness reported so far for pure-blue PeLEDs. Furthermore, the PeLEDs exhibit robust durability, with a half-lifetime exceeding 12 h under continuous operation, representing a record performance value for blue PeLEDs.

Perovskite Quantum Dots with Ultralow Trap Density by Acid Etching-Driven Ligand Exchange for High Luminance and Stable Pure-Blue Light-Emitting Diodes

This article offers a materials-chemistry perspective for colloidal quantum dots (QDs) in the field of display, including QD-enhanced liquid-crystal-display (QD-LCD) and QD-based light-emitting-diodes (QLEDs) display. The rapid successes of QDs for display in the past five years are not accidental but have a deep root in both maturity of their synthetic chemistry and their unique chemical, optical, and optoelectronic properties. This article intends to discuss the natural match of QD emitters for display and chemical means to eventually bring about their full potential.

Quantum Dots for Display Applications.

Outstanding photoluminescence (PL) and electroluminescence properties of quantum dots (QDs) promise possibilities for them to meet challenging expectations of electrochemiluminescence (ECL), which ...

Quantum Dots with Highly Efficient, Stable, and Multicolor Electrochemiluminescence.

Aliphatic carboxylates are the most common class of surface ligands to stabilize colloidal nanocrystals. The widely used approach to identify the coordination modes between surface cationic sites and carboxylate ligands is based on the empirical infrared (IR) spectroscopic assignment, which is often ambiguous and thus hampers the practical control of surface structures. In this report, multiple techniques based on nuclear magnetic resonance (NMR) and IR spectra are applied to distinguish the different coordination structures in a series of zinc-blende CdSe nanocrystals with unique facet structures, including nanoplatelets dominated with {100} basal planes, hexahedrons with only three types of low-index facets (i.e., {100}, {110}, and {111}), and spheroidal dots without well-defined facets. Interpretation and assignment of NMR and IR signals were assisted by density functional theory (DFT) calculations. In addition to the identification of facet-sensitive bonding modes, the present methods also allow a nondestructive quantification of mixed ligands.

Yufei Shu

Papers

Electrochemically-stable ligands bridge the photoluminescence-electroluminescence gap of quantum dots.

Quantum Dots for Display Applications.

Quantum Dots with Highly Efficient, Stable, and Multicolor Electrochemiluminescence.

Identification of Facet-Dependent Coordination Structures of Carboxylate Ligands on CdSe Nanocrystals

Quantum Dots for Display