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1.
Adv Sci (Weinh) ; 11(34): e2306167, 2024 Sep.
Artículo en Inglés | MEDLINE | ID: mdl-38992965

RESUMEN

Quasi-2D perovskites light-emitting diodes (PeLEDs) have achieved significant progress due to their superior optical and electronic properties. However, the blue PeLEDs still exist inefficient energy transfer and electroluminescence performance caused by mixed multidimensional phase distribution. In this work, transition metal salt (zinc bromide, ZnBr2) is introduced to modulate phase distributions by suppressing the nucleation of high n phase perovskites, which effectively shortens the energy transfer path for blue emission. Moreover, ZnBr2 also facilitates energy level matching and reduces non-radiative recombination, thus improving electroluminescence (EL) efficiency. Benefiting from these combined improvements, an efficient blue PeLEDs is obtained with a maximum external quantum efficiency (EQE) of 16.2% peaking located at 486 nm. This work provides a promising approach to tune phase distribution of quasi-2D perovskites and achieving highly efficient blue PeLEDs.

2.
ACS Appl Mater Interfaces ; 14(41): 46857-46865, 2022 Oct 19.
Artículo en Inglés | MEDLINE | ID: mdl-36149762

RESUMEN

Mixed-halide (Cl and Br) perovskite nanocrystals (NCs) are of particular interest because they hold great potential for use in high-efficiency blue light-emitting diodes (LEDs). Generally, mixed-halide compounds are obtained by either a one-step synthesis with simultaneous addition of both halide precursors or a postsynthetic anion exchange using the opposite halogen. However, both strategies fail to prevent the formation of deep-level Cl vacancy defects, rendering the photoluminescence quantum yields (PLQYs) typically lower than 30%. Here, by optimizing both thermodynamic and kinetic processes, we devise a two-step hot-injection approach, which simultaneously realizes Cl vacancy filling and efficient anion exchange between Cl- and Br-. Both the identity of Br precursors and their injection temperature are revealed to be critical in transforming those highly defective CsPbCl3 NCs to defect-free CsPb(Cl/Br)3. The optimally synthesized NCs exhibit a saturated blue emission at ∼460 nm with a near-unity PLQY and a narrow emission bandwidth of 18 nm, which represents one of the most efficient blue emitters reported so far. The turn-on voltage of the ensuing LEDs is ∼4.0 V, which is lower than those of most other mixed-halide perovskites. In addition, LEDs exhibit a stable electroluminescence peak at 460 nm under a high bias voltage of 8.0 V. We anticipate that our findings will provide new insights into the materials design strategies for producing high-optoelectronic-quality Cl-containing perovskites.

3.
Small ; 18(15): e2108120, 2022 04.
Artículo en Inglés | MEDLINE | ID: mdl-35253372

RESUMEN

InP quantum dots (QDs) have attracted much attention owing to their nontoxic properties and shown great potential in optoelectronic applications. Due to the surface defects and lattice mismatch, the interfacial structure of InP/ZnS QDs plays a significant role in their performance. Herein, the formation of In-S and Sx -In-P1-x interlayers through anion exchange at the shell-growth stage is revealed. More importantly, it is proposed that the composition of interface is dependent on the synergistic effect of halogen ions and shelling temperature. High shelling temperature contributes to the optical performance improvement resulting from the formation of interlayers, besides the thicker ZnS shell. Moreover, the effect relates to the halogen ions where I- presents more obvious enhancement than Br- and Cl- , owing to their different ability to coordinate with In dangling bonds, which are inclined to form In-S and Sx -In-P1-x bonds. Further, the anion exchange under I- -rich environment causes a blue-shift of emission wavelength with shelling temperature increasing, unobserved in a Cl- - or Br- -rich environment. It contributes to the preparation of highly efficient blue emissive InP/ZnS QDs with emission wavelength of 473 nm, photoluminescence quantum yield of ≈50% and full width at half maximum of 47 nm.


Asunto(s)
Puntos Cuánticos , Halógenos , Puntos Cuánticos/química , Sulfuros/química , Temperatura , Compuestos de Zinc
4.
Environ Sci Pollut Res Int ; 29(37): 56684-56695, 2022 Aug.
Artículo en Inglés | MEDLINE | ID: mdl-35347616

RESUMEN

Sunlight active blue emissive zirconium, nitrogen, and sulfur co-doped carbon dots (Zr-N-S-CDs) have been synthesized by microwave-induced pyrolysis for achieving efficient photocatalytic degradation of pollutant malachite green dye (MG) in water. Surface morphology studies using high-resolution transmission electron microscopy confirmed the formation of spherical-shaped CDs with an absorbance peak at 350 nm and emission peak at 437 nm in UV-vis and fluorescence spectroscopy, respectively. Surface functional groups, elemental composition, and metal/non-metal co-doping were confirmed by Fourier transform infrared spectroscopy and X-ray photoelectron spectroscopy. To understand the photocatalytic performance of Zr-N-S-CDs, various parameters, such as the source of energy, concentration of dye, catalyst dosage, and change in pH, were investigated. MG dye (20 ppm) at a pH 7 with 0.5 mg/mL of Zr-N-S-CDs could be photodegraded efficiently in 90 min under sunlight (99%) compared to dark and artificial light conditions. Moreover, real-time analysis of degradation rate could be conveniently calculated by integrating the colorimetric responses of MG dye with RGB values obtained by the "Color Picker" app of a smartphone. The degradation rate obtained using a smartphone (97.89%) was found to be in agreement with the UV-vis spectroscopy (99%), thus, providing a new, handy, and instrument-free route for speedy and quantitative estimation of the degradation of hazardous MG dye by Zr-N-S-CDs.


Asunto(s)
Carbono , Agua , Carbono/química , Colorantes , Nitrógeno/química , Espectroscopía de Fotoelectrones , Colorantes de Rosanilina , Teléfono Inteligente , Azufre/química , Agua/química , Circonio/química
5.
ACS Nano ; 14(10): 13246-13255, 2020 Oct 27.
Artículo en Inglés | MEDLINE | ID: mdl-32910640

RESUMEN

A series of poly(fluorene-co-phenylene)-based anionic conjugated polyelectrolytes (CPEs) are prepared with varying sizes of counterions (tetramethylammonium, tetraethylammonium, and tetrabutylammonium (TBA+)) and studied as a hole-transporting layer (HTL) for sky-blue-emissive perovskite light-emitting diodes (PeLEDs). Ionic CPE HTLs improve the wettability, compatibility, and nucleation of perovskite crystals at interfaces, enabling highly crystalline perovskite crystal growth with enhanced light-emitting properties. By incorporating the CPE HTLs containing bulky TBA+ counterions (MPS2-TBA) in place of PEDOT:PSS, the decreased phonon-electron coupling and increased exciton binding energy in perovskites are measured by temperature-dependent photoluminescence (PL) measurements. By increasing the size of counterions in CPE interlayers, the PL intensities and lifetimes of perovskite films increase. Through space-charge-limited current measurements, the lowest trap density is measured in the perovskite film on MPS2-TBA, emphasizing a critical role of larger counterions. Using density functional theory, MPS2-TBA is calculated to show the strongest adsorption affinity toward the interstitial defect of lead ions, explaining its pronounced interfacial defect passivation. The counterion size in CPE interlayers is interpreted as a main factor to determine the adsorption affinity onto perovskite, which determines the interacted area as noncovalent adsorption occurs. Finally, the sky-blue-emissive quasi-2D PeLED with MPS2-TBA shows the highest luminance efficiency (a peak EQE of 2.6% at 489 nm) and significantly improved spectral stability.

6.
Angew Chem Int Ed Engl ; 59(49): 22156-22162, 2020 Dec 01.
Artículo en Inglés | MEDLINE | ID: mdl-32803819

RESUMEN

Quasi-two-dimensional (2D) perovskites are promising candidates for light generation owing to their high radiative rates. However, strong exciton-phonon interactions caused by mechanical softening of the surface act as a bottleneck in improving their suitability for a wide range of lighting and display applications. Moreover, it is not easily available to tune the phonon interactions in bulk films. Here, we adopt bottom-up fabricated blue emissive perovskite nanoplatelets (NPLs) as model systems to elucidate and as well as tune the phonon interactions via engineering of binary NPL solids. By optimizing component domains, the phonon coupling strength can be reduced by a factor of 2 driven by the delocalization of 2D excitons in out-of-plane orientations. It shows the picosecond energy transfer originated from the Förster resonance energy transfer (FRET) efficiently competes with the exciton-phonon interactions in the binary system.

7.
Molecules ; 24(22)2019 Nov 08.
Artículo en Inglés | MEDLINE | ID: mdl-31717285

RESUMEN

Hybrid white organic light-emitting diodes (WOLEDs) have drawn great attention both for display and solid-state lighting purposes because of the combined advantages of desirable stability of fluorescent dyes and high efficiency of phosphorescent materials. However, in most WOLEDs, obtaining high efficiency often requires complex device structures. Herein, we achieved high-efficiency hybrid WOLEDs using a simple but efficacious structure, which included a non-doped blue emissive layer (EML) to separate the exciton recombination zone from the light emission region. After optimization of the device structure, the WOLEDs showed a maximum power efficiency (PE), current efficiency (CE), and external quantum efficiency (EQE) of 82.3 lm/W, 70.0 cd/A, and 22.2%, respectively. Our results presented here provided a new option for promoting simple-structure hybrid WOLEDs with superior performance.


Asunto(s)
Luz , Modelos Teóricos
8.
Molecules ; 22(9)2017 Sep 05.
Artículo en Inglés | MEDLINE | ID: mdl-28872608

RESUMEN

A new type of blue emitter, N²-Indolyl-1,2,3-triazoles (NITs), with the λmax ranging from 420-480 nm and the Stokes shift from 89-143 nm, were synthesized through the coupling reaction of indoles with triazole derivatives. The influence of different substitution patterns on the optical properties (efficiency, excitation, and emission wavelengths) of the NITs was investigated. In addition, one palladium complex were synthesized by using NITs as the ligands, which, however, exhibited no fluorescent activity, but did show the enhanced co-planarity. Lastly, two bio-active molecule derivatives were explored for the potential use of these novel dyes in related chemical and biological applications.


Asunto(s)
Complejos de Coordinación/química , Colorantes Fluorescentes/química , Indoles/química , Paladio/química , Triazoles/química , Complejos de Coordinación/síntesis química , Fluorescencia , Colorantes Fluorescentes/síntesis química , Indoles/síntesis química , Ligandos , Espectroscopía de Resonancia Magnética , Espectrometría de Masas , Triazoles/síntesis química
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