Showing papers on "Photoluminescence published in 2022"

Single‐Junction Organic Solar Cells with 19.17% Efficiency Enabled by Introducing One Asymmetric Guest Acceptor

Abstract: The ternary strategy has been widely identified as an effective approach to obtain high‐efficiency organic solar cells (OSCs). However, for most ternary OSCs, the nonradiative voltage loss lies between those of the two binary devices, which limits further efficiency improvements. Herein, an asymmetric guest acceptor BTP‐2F2Cl is designed and incorporated into a PM1:L8‐BO host blend. Compared with the L8‐BO neat film, the L8‐BO:BTP‐2F2Cl blend film shows higher photoluminescence quantum yield and larger exciton diffusion length. Introducing BTP‐2F2Cl into the host blend extends its absorption spectrum, improves the molecular packing of host materials, and suppresses the nonradiative charge recombination of the ternary OSCs. Consequently, the power conversion efficiency is improved up to 19.17% (certified value 18.7%), which represents the highest efficiency value reported for single‐junction OSCs so far. The results show that improving the exciton behaviors is a promising approach to reducing the nonradiative voltage loss and realizing high‐performance OSCs.

A multifunctional chemical toolbox to engineer carbon dots for biomedical and energy applications

Abstract: Photoluminescent carbon nanoparticles, or carbon dots, are an emerging class of materials that has recently attracted considerable attention for biomedical and energy applications. They are defined by characteristic sizes of <10 nm, a carbon-based core and the possibility to add various functional groups at their surface for targeted applications. These nanomaterials possess many interesting physicochemical and optical properties, which include tunable light emission, dispersibility and low toxicity. In this Review, we categorize how chemical tools impact the properties of carbon dots. We look for pre- and postsynthetic approaches for the preparation of carbon dots and their derivatives or composites. We then showcase examples to correlate structure, composition and function and use them to discuss the future development of this class of nanomaterials. This Review discusses synthetic strategies to functionalize photoluminescent carbon nanomaterials, or carbon dots, for targeted applications.

Efficient selenium-integrated TADF OLEDs with reduced roll-off

Abstract: Organic light emitters based on multiresonance-induced thermally activated delayed fluorescent materials have great potential for realizing efficient, narrowband organic light-emitting diodes (OLEDs). However, at high brightness operation, efficiency roll-off attributed to the slow reverse intersystem crossing (RISC) process hinders the use of multiresonance-induced thermally activated delayed fluorescent materials in practical applications. Here we report a heavy-atom incorporating emitter, BNSeSe, which is based on a selenium-integrated boron–nitrogen skeleton and exhibits 100% photoluminescence quantum yield and a high RISC rate (kRISC) of 2.0 × 106 s−1. The corresponding green OLEDs exhibit excellent external quantum efficiencies of up to 36.8% and ultra-low roll-off character at high brightnesses (with very small roll-off values of 2.8% and 14.9% at 1,000 cd m−2 and 10,000 cd m−2, respectively). Furthermore, the outstanding capability to harvest triplet excitons also enables BNSeSe to be a superior sensitizer for a hyperfluorescence OLED, which shows state-of-the-art performance with a high excellent external quantum efficiency of 40.5%, power efficiency beyond 200 lm W−1, and luminance close to 20,0000 cd m−2. Green OLEDs based on BNSeSe offer high operational efficiency and reduced efficiency roll-off.

Compact ultrabroadband light-emitting diodes based on lanthanide-doped lead-free double perovskites

Abstract: Abstract Impurity doping is an effective approach to tuning the optoelectronic performance of host materials by imparting extrinsic electronic channels. Herein, a family of lanthanide (Ln 3+ ) ions was successfully incorporated into a Bi:Cs 2 AgInCl 6 lead-free double-perovskite (DP) semiconductor, expanding the spectral range from visible (Vis) to near-infrared (NIR) and improving the photoluminescence quantum yield (PLQY). After multidoping with Nd, Yb, Er and Tm, Bi/Ln:Cs 2 AgInCl 6 yielded an ultrabroadband continuous emission spectrum with a full width at half-maximum of ~365 nm originating from intrinsic self-trapped exciton recombination and abundant 4f–4f transitions of the Ln 3+ dopants. Steady-state and transient-state spectra were used to ascertain the energy transfer and emissive processes. To avoid adverse energy interactions between the various Ln 3+ ions in a single DP host, a heterogeneous architecture was designed to spatially confine different Ln 3+ dopants via a “DP-in-glass composite” (DiG) structure. This bottom-up strategy endowed the prepared Ln 3+ -doped DIG with a high PLQY of 40% (nearly three times as high as that of the multidoped DP) and superior long-term stability. Finally, a compact Vis–NIR ultrabroadband (400~2000 nm) light source was easily fabricated by coupling the DiG with a commercial UV LED chip, and this light source has promising applications in nondestructive spectroscopic analyses and multifunctional lighting.

Compact ultrabroadband light-emitting diodes based on lanthanide-doped lead-free double perovskites

Abstract: Abstract Impurity doping is an effective approach to tuning the optoelectronic performance of host materials by imparting extrinsic electronic channels. Herein, a family of lanthanide (Ln 3+ ) ions was successfully incorporated into a Bi:Cs 2 AgInCl 6 lead-free double-perovskite (DP) semiconductor, expanding the spectral range from visible (Vis) to near-infrared (NIR) and improving the photoluminescence quantum yield (PLQY). After multidoping with Nd, Yb, Er and Tm, Bi/Ln:Cs 2 AgInCl 6 yielded an ultrabroadband continuous emission spectrum with a full width at half-maximum of ~365 nm originating from intrinsic self-trapped exciton recombination and abundant 4f–4f transitions of the Ln 3+ dopants. Steady-state and transient-state spectra were used to ascertain the energy transfer and emissive processes. To avoid adverse energy interactions between the various Ln 3+ ions in a single DP host, a heterogeneous architecture was designed to spatially confine different Ln 3+ dopants via a “DP-in-glass composite” (DiG) structure. This bottom-up strategy endowed the prepared Ln 3+ -doped DIG with a high PLQY of 40% (nearly three times as high as that of the multidoped DP) and superior long-term stability. Finally, a compact Vis–NIR ultrabroadband (400~2000 nm) light source was easily fabricated by coupling the DiG with a commercial UV LED chip, and this light source has promising applications in nondestructive spectroscopic analyses and multifunctional lighting.

High‐Performance Narrowband Pure‐Red OLEDs with External Quantum Efficiencies up to 36.1% and Ultralow Efficiency Roll‐Off

Abstract: High‐color‐purity blue and green organic light‐emitting diodes (OLEDs) have been resolved thanks to the development of B/N‐based polycyclic multiple resonance (MR) emitters. However, due to the derivatization limit of B/N polycyclic structures, the design of red MR emitters remains challenging. Herein, a series of novel red MR emitters is reported by para‐positioning N–π–N, O–π–O, B–π–B pairs onto a benzene ring to construct an MR central core. These emitters can be facilely and modularly synthesized, allowing for easy fine‐tuning of emission spectra by peripheral groups. Moreover, these red MR emitters display excellent photophysical properties such as near‐unity photoluminescence quantum yield (PLQY), fast radiative decay rate (kr) up to 7.4 × 107 s−1, and most importantly, narrowband emission with full‐width at half‐maximum (FWHM) of 32 nm. Incorporating these MR emitters, pure red OLEDs sensitized by phosphor realize state‐of‐the‐art device performances with external quantum efficiency (EQE) exceeding 36%, ultralow efficiency roll‐off (EQE remains as high as 25.1% at the brightness of 50 000 cd m−2), ultrahigh brightness over 130 000 cd m−2, together with good device lifetime.

Electron–phonon coupling-assisted universal red luminescence of o-phenylenediamine-based carbon dots

Abstract: Abstract Due to the complex core–shell structure and variety of surface functional groups, the photoluminescence (PL) mechanism of carbon dots (CDs) remain unclear. o-Phenylenediamine (oPD), as one of the most common precursors for preparing red emissive CDs, has been extensively studied. Interestingly, most of the red emission CDs based on oPD have similar PL emission characteristics. Herein, we prepared six different oPD-based CDs and found that they had almost the same PL emission and absorption spectra after purification. Structural and spectral characterization indicated that they had similar carbon core structures but different surface polymer shells. Furthermore, single-molecule PL spectroscopy confirmed that the multi-modal emission of those CDs originated from the transitions of different vibrational energy levels of the same PL center in the carbon core. In addition, the phenomenon of “spectral splitting” of single-particle CDs was observed at low temperature, which confirmed these oPD-based CDs were unique materials with properties of both organic molecules and quantum dots. Finally, theoretical calculations revealed their potential polymerization mode and carbon core structure. Moreover, we proposed the PL mechanism of red-emitting CDs based on oPD precursors; that is, the carbon core regulates the PL emission, and the polymer shell regulates the PL intensity. Our work resolves the controversy on the PL mechanism of oPD-based red CDs. These findings provide a general guide for the mechanism exploration and structural analysis of other types of CDs.

Electron–phonon coupling-assisted universal red luminescence of o-phenylenediamine-based carbon dots

Abstract: Abstract Due to the complex core–shell structure and variety of surface functional groups, the photoluminescence (PL) mechanism of carbon dots (CDs) remain unclear. o-Phenylenediamine (oPD), as one of the most common precursors for preparing red emissive CDs, has been extensively studied. Interestingly, most of the red emission CDs based on oPD have similar PL emission characteristics. Herein, we prepared six different oPD-based CDs and found that they had almost the same PL emission and absorption spectra after purification. Structural and spectral characterization indicated that they had similar carbon core structures but different surface polymer shells. Furthermore, single-molecule PL spectroscopy confirmed that the multi-modal emission of those CDs originated from the transitions of different vibrational energy levels of the same PL center in the carbon core. In addition, the phenomenon of “spectral splitting” of single-particle CDs was observed at low temperature, which confirmed these oPD-based CDs were unique materials with properties of both organic molecules and quantum dots. Finally, theoretical calculations revealed their potential polymerization mode and carbon core structure. Moreover, we proposed the PL mechanism of red-emitting CDs based on oPD precursors; that is, the carbon core regulates the PL emission, and the polymer shell regulates the PL intensity. Our work resolves the controversy on the PL mechanism of oPD-based red CDs. These findings provide a general guide for the mechanism exploration and structural analysis of other types of CDs.

Highly efficient emission and high-CRI warm white light-emitting diodes from ligand-modified CsPbBr&lt;sub&gt;3&lt;/sub&gt; quantum dots

Abstract: All-inorganic CsPbBr₃ perovskite quantum dots (QDs) have received great attention in white light emission because of their outstanding properties. However, their practical application is hindered by poor stability. Herein, we propose a simple strategy to synthesize excellent stability and efficient emission of CsPbBr₃ QDs by using 2-hexyldecanoic acid (DA) as a ligand to replace the regular oleic acid (OA) ligand. Thanks to the strong binding energy between DA ligand and QDs, the modified QDs not only show a high photoluminescence quantum yield (PLQY) of 96% but also exhibit high stability against ethanol and water. Thereby warm white light-emitting diodes (WLEDs) are constructed by combining ligand modified CsPbBr₃ QDs with red AgInZnS QDs on blue emitting InGaN chips, exhibiting a color rendering index of 93, a power efficiency of 64.8 lm/W, a CIE coordinate of (0.44, 0.42) and correlated color temperature value of 3018 K. In addition, WLEDs based on ligand modified CsPbBr₃ QDs also exhibit better thermal performance than that of WLEDs based on the regular CsPbBr₃ QDs. The combination of improved efficiency and better thermal stability with high color quality indicates that the modified CsPbBr₃ QDs are ideal for WLEDs application.

Colloidal Metal‐Halide Perovskite Nanoplatelets: Thickness‐Controlled Synthesis, Properties, and Application in Light‐Emitting Diodes

Abstract: Colloidal metal-halide perovskite nanocrystals (MHP NCs) are gaining significant attention for a wide range of optoelectronics applications owing to their exciting properties, such as defect tolerance, near-unity photoluminescence quantum yield, and tunable emission across the entire visible wavelength range. Although the optical properties of MHP NCs are easily tunable through their halide composition, they suffer from light-induced halide phase segregation that limits their use in devices. However, MHPs can be synthesized in the form of colloidal nanoplatelets (NPls) with monolayer (ML)-level thickness control, exhibiting strong quantum confinement effects, and thus enabling tunable emission across the entire visible wavelength range by controlling the thickness of bromide or iodide-based lead-halide perovskite NPls. In addition, the NPls exhibit narrow emission peaks, have high exciton binding energies, and a higher fraction of radiative recombination compared to their bulk counterparts, making them ideal candidates for applications in light-emitting diodes (LEDs). This review discusses the state-of-the-art in colloidal MHP NPls: synthetic routes, thickness-controlled synthesis of both organic-inorganic hybrid and all-inorganic MHP NPls, their linear and nonlinear optical properties (including charge-carrier dynamics), and their performance in LEDs. Furthermore, the challenges associated with their thickness-controlled synthesis, environmental and thermal stability, and their application in making efficient LEDs are discussed.

ZnO size and shape effect on antibacterial activity and cytotoxicity profile

Abstract: Abstract The aim of our work was the synthesis of ZnO nano- and microparticles and to study the effect of shapes and sizes on cytotoxicity towards normal and cancer cells and antibacterial activity toward two kinds of bacteria. We fabricated ZnO nano- and microparticles through facile chemical and physical routes. The crystal structure, morphology, textural properties, and photoluminescent properties were characterized by powder X-ray diffraction, electron microscopies, nitrogen adsorption/desorption measurements, and photoluminescence spectroscopy. The obtained ZnO structures were highly crystalline and monodispersed with intensive green emission. ZnO NPs and NRs showed the strongest antibacterial activity against Escherichia coli and Staphylococcus aureus compared to microparticles due to their high specific surface area. However, the ZnO HSs at higher concentrations also strongly inhibited bacterial growth. S. aureus strain was more sensitive to ZnO particles than the E. coli. ZnO NPs and NRs were more harmful to cancer cell lines than to normal ones at the same concentration.

Achieving 37.1% Green Electroluminescent Efficiency and 0.09 eV Full Width at Half Maximum Based on a Ternary Boron-Oxygen-Nitrogen Embedded Polycyclic Aromatic System.

Abstract: Herein, a ternary boron-oxygen-nitrogen embedded polycyclic aromatic hydrocarbon with multiple resonance thermally activated delayed fluorescence (MR-TADF), namely DBNO, is developed by adopting the para boron-π-boron and para oxygen-π-oxygen strategy. The designed molecule presents a vivid green emission with high photoluminescence quantum yield (96%) and extremely narrow full width at half maximum (FWHM) of 19 nm/0.09 eV, which surpasses all previously reported green TADF emitters to date. In addition, the long molecular structure along the transition dipole moment direction endows it with a high horizontal emitting dipole ratio of 96%. The organic light-emitting diode (OLED) based on DBNO reveals a narrowband green emission with a peak at 504 nm and a FWHM of 24 nm/0.12 eV. Particularly, a significantly improved device performance is achieved by the TADF-sensitization ( hyperfluorescence ) mechanism, presenting a FWHM of 27 nm and maximum external quantum efficiency of 37.1%.

Bridging Effect of S-C Bond for Boosting Electron Transfer over Cubic Hollow CoS/g-C3N4 Heterojunction toward Photocatalytic Hydrogen Production.

Abstract: The construction of interfacial effects and chemical bonds between catalysts is one of the effective strategies to facilitate photogenerated electron transfer. A novel hollow cubic CoS is derived from Co-ZIF-9 and the S-C bond is successfully constructed between CoS and g-C3N4. The S-C bond acts as a bridge for electronic transmission, allowing the rapid transmission of photoelectron to hydrogen evolution active site in CoS. In addition, the results of electrochemical impedance spectroscopy and time-resolved photoluminescence spectroscopy show that the S-C bond acts as a bridge to quickly transfer photogenerated carriers in the composite material, and achieves the effect of high-efficiency hydrogen evolution. The hydrogen production of SgZ-45 reaches 9545 μmol·g-1 in 5 h, which is 53 and 12 times that of g-C3N4 and ZIF-9, respectively. The intrinsic mechanism of photoelectron transfer through S-C bonds can be further confirmed by density functional theory (DFT) calculations. This work provides new insights for building a chemical bond electron transfer bridge between MOF derivatives and nonmetallic photocatalytic materials.

On-demand modulating afterglow color of water-soluble polymers through phosphorescence FRET for multicolor security printing

Abstract: Developing full-color organic ultralong room temperature phosphorescence (OURTP) materials with continuously variable afterglow emission is of considerable practical importance in diverse optoelectronic applications but remains a formidable challenge. Here, we present an effective strategy for on-demand engineering of afterglow color in water-soluble polymeric systems via efficient phosphorescence Förster resonance energy transfer. Using a blue afterglow emitting water-soluble polymer as host and a series of fluorescent emitters with varied emissive colors as guests, afterglow emission is rationally modulated, conferring the full-color afterglow emission ranging from blue to red and even white with ultralong lifetimes up to 4.2 s and photoluminescence quantum yields of 36%.These water-soluble multicolor-emitting polymeric afterglow systems can function as OURTP security inks, and multilevel information encryption was successfully established by RGB-based multicolor security printing. These results present important guidance in developing high-performance afterglow polymers with on-demand color tuning ability for remarkable optoelectronic applications.

Ambipolar Self‐Host Functionalization Accelerates Blue Multi‐Resonance Thermally Activated Delayed Fluorescence with Internal Quantum Efficiency of 100%

Abstract: Emerging multi‐resonance (MR) thermally activated delayed fluorescence (TADF) emitters can combine 100% exciton harvesting and high color purity for their organic light‐emitting diodes (OLED). However, the highly planar configurations of MR molecules lead to intermolecular‐interaction‐induced quenching. A feasible way is integrating host segments into MR molecules, namely a “self‐host” strategy, but without involving additional charge transfer and/or vibrational components to excited states. Herein, an ambipolar self‐host featured MR emitter, tCBNDADPO, is demonstrated, whose ambipolar host segment (DADPO) significantly and comprehensively improves the TADF properties, especially greatly accelerated singlet radiative rate constant of 2.11 × 108 s−1 and exponentially reduced nonradiative rate constants. Consequently, at the same time as preserving narrowband blue emission with an FWHM of ≈28 nm at a high doping concentration of 30%, tCBNDADPO reveals state‐of‐the‐art photoluminescence and electroluminescence quantum efficiencies of 99% and 30%, respectively. The corresponding 100% internal quantum efficiency of tCBNDADPO supported by an ultrasimple trilayer and heavily doped device demonstrates the feasibility of the ambipolar self‐host strategy for constructing practically applicable MR materials.

Controlling the nucleation and growth kinetics of lead halide perovskite quantum dots

Abstract: Colloidal lead halide perovskite nanocrystals are of interest as photoluminescent quantum dots (QDs) whose properties depend on the size and shape. They are normally synthesized on subsecond time scales through hard-to-control ionic metathesis reactions. We report a room-temperature synthesis of monodisperse, isolable, spheroidal APbBr3 QDs (“A” indicates cesium, formamidinium, and methylammonium) that are size tunable from 3 to >13 nanometers. The kinetics of both nucleation and growth are temporally separated and substantially slowed down by the intricate equilibrium between the precursor (PbBr2) and the A[PbBr3] solute, with the latter serving as a monomer. QDs of all these compositions exhibit up to four excitonic transitions in their linear absorption spectra, and we demonstrate that the size-dependent confinement energy for all transitions is independent of the A-site cation. Description Slowing nanoparticle growth Inorganic materials with more covalent bonding, such as cadmium selenide, form uniform nanoparticles under fast growth conditions, but perovskites such as cesium lead bromide (CsPbBr3) are more ionic and grow rapidly to form larger nanoparticles. Akkerman et al. controlled the nanoparticles’ growth kinetics by using trioctylphosphine oxide, which solubilized the PbBr2 precursor, bound to the cation-[PbBr3] monomer (solute), and weakly coordinated to the crystal nuclei surfaces. Nanoparticles with diameters from 3 to 13 nanometers were stabilized and isolated in high yield with lecithin, a long-chain zwitterion. Four well-resolved excitonic transitions with size-dependent confinement energies were seen for cesium as well as organic cations. —PDS Monodisperse lead-halide perovskite nanocrystals are synthesized through slow and temporally separated nucleation and growth.

Yellow‐Emissive Carbon Dots with High Solid‐State Photoluminescence

Abstract: Carbon dots (CDs) present an enticing prospect for a variety of optical applications relying on their high photoluminescence (PL) quantum yield (QY). Herein, the synthesis, optical properties, structural characterizations, density‐functional theory (DFT) calculations, and potential applications of yellow‐emissive CDs (Y‐CDs) with ultra‐high PL QY are reported. Solvothermal treatment of citric acid and urea in toluene, followed by column chromatography, produces Y‐CDs exhibiting excitation‐independent PL emission at 553 nm with a high solution PL QY of 92%. A variety of optical and structural characterizations and DFT theoretical calculations are implemented to confirm the general structure and fluorescence origin of Y‐CDs, conjugated sp2‐carbon domains (fused rings) with edge groups. Significantly, transparent Y‐CDs/acrylic resin films with strong solid‐state emissions are fabricated. The Y‐CD films exhibit a high fluorescence with PL QY of 98%, good PL stability (no PL variation under continuous irradiation for 180 h), and large Stokes shift (129 nm). The potential applications of Y‐CDs for luminescent solar concentrators as well as yellow phosphors for lighting are also demonstrated. These findings thus promote the development of high‐performance CDs and their optoelectronic applications.

Large-Area Perovskite-Related Copper Halide Film for High-Resolution Flexible X-ray Imaging Scintillation Screens

Abstract: Flexible copper halide films of 400 cm2 area were fabricated with outstanding mechanical stability, excellent film uniformity, nearly 100% photoluminescence quantum yields, and resistance to water and heat. The re-absorption-free X-ray imaging scintillators engineered based on these films exhibit superior scintillation performance with a detection limit as low as 48.6 nGy/s and 17 lp/mm X-ray imaging resolution, representing the highest imaging resolution for powder-based screens.

Red Perovskite Light‐Emitting Diodes with Efficiency Exceeding 25% Realized by Co‐Spacer Cations

Abstract: Perovskite light-emitting diodes (PeLEDs) have received great attention in recent years due to their narrow emission bandwidth and tunable emission spectrum. Efficient red emission is one of most important parts for lighting and displays. Quasi-2D perovskites can deliver high emission efficiency due to the strong carrier confinement, while the external quantum efficiencies (EQE) of red quasi-2D PeLEDs are inefficient at present, which is due to the complex distribution of different n-value phases in quasi-2D perovskite films. In this work, the phase distribution of the quasi-2D perovskite is finely controlled by mixing two different large organic cations, which effectively reduces the amount of smaller n-index phases, meanwhile the passivation of lead and halide defects in perovskite films is realized. Accordingly, the PeLEDs show 25.8% EQE and 1300 cd m−2 maximum brightness at 680 nm, which exhibits the highest performance for red PeLEDs up to now.