Cesium lead halide (CsPbX) perovskite nanocrystals (NCs) have demonstrated extremely excellent optical properties and great application potentials in various optoelectronic devices. However, because of the anion exchange, it is difficult to achieve white-light and multicolor emission for practical applications. Herein, we present the successful doping of various lanthanide ions (Ce, Sm, Eu, Tb, Dy, Er, and Yb) into the lattices of CsPbCl perovskite NCs through a modified hot-injection method. For the lanthanide ions doped perovskite NCs, high photoluminescence quantum yield (QY) and stable and widely tunable multicolor emissions spanning from visible to near-infrared (NIR) regions are successfully obtained. This work indicates that the doped perovskite NCs will inherit most of the unique optical properties of lanthanide ions and deliver them to the perovskite NC host, thus endowing the family of perovskite materials with excellent optical, electric, or magnetic properties.
Intracellular pH sensing is of importance and can be used as an indicator for monitoring the evolution of various diseases and the health of cells. Here, we developed a new class of surface-functionalized MXene quantum dots (QDs), TiC, by the sonication cutting and hydrothermal approach and further explored their intracellular pH sensing. The functionalized TiC QDs exhibit bright excitation-dependent blue photoluminescence (PL) originating from the size effect and surface defects. Meanwhile, TiC QDs demonstrate a high PL response induced by the deprotonation of the surface defects. Furthermore, combining the highly pH sensitive TiC QDs with the pH insensitive [Ru(dpp)]Cl, we developed a ratiometric pH sensor to quantitatively monitor the intracellular pH values. These novel MXene quantum dots can serve as a promising platform for developing practical fluorescent nanosensors.
Carbon dots (CDs) have emerged as novel fluorescent probes due to their remarkable optical properties; however, red emission is still rare, has a relatively low efficiency, and its mechanism remains ambiguous. Herein, relatively efficient red-emission CDs based on p-phenylenediamine were prepared through various solvothermal means, where the highest quantum yield approached 41.1% in n-amyl alcohol, which was the most efficient quantum yield reported to date. Various structural characterizations were performed and confirmed that the red emission originated from the molecular states consisting of a nitrogen-containing organic fluorophore. The CDs were dispersed in different organic solvents and showed tunable emission, evolving from green to orange-red in aprotic solvents and a red emission in protic solvents. Further solvent correlation studies indicated that the hydrogen bond effect between the CDs and solvents was the main mechanism leading to the spectral shift. Accordingly, solid-state luminescent CDs-polymers were fabricated, which also demonstrated continuously tunable emission properties. This work opens a new window for recognizing the generation of tunable and red-emission CDs.
Colloidal perovskite nanocrystals (NCs), especially the fully inorganic cesium lead halide (CsPbX, X = Cl, Br, I) NCs, have been considered as promising candidates for lighting and display applications due to their narrow band emission, tunable band gap and high photoluminescence quantum yields (QYs). However, owing to the anion exchange in the CsPbX NCs, stable multi-color and white light emissions are difficult to achieve, thus limiting their practical optoelectronic applications. In this work, dual ion Bi/Mn codoped CsPbCl perovskite NCs were prepared through the hot injection method for the first time to the best of our knowledge. Through simply adjusting the doping ion concentrations, the codoped NCs exhibited tunable emissions spanning the wide range of correlated color temperature (CCT) from 19 000 K to 4250 K under UV excitation. This interesting spectroscopic behaviour benefits from efficient energy transfer from the perovskite NC host to the intrinsic energy levels of Bi or Mn doping ions. Finally, taking advantage of the cooperation between the excitonic transition of the CsPbCl perovskite NC host and the intrinsic emissions from Bi and Mn ions, white light emission with the Commission Internationale de l'Eclairage (CIE) color coordinates of (0.33, 0.29) was developed in the codoped CsPbCl NCs.
The performance of perovskite solar cells (PSCs) strongly depends on the electron transport layer (ETL), perovskite absorber, hole transport layer (HTL), and their interfaces. Herein, the first approach to utilize ultrathin 2D titanium‐carbide MXenes (Ti3C2Tx quantum dots, TQD) by engineering the perovskite/TiO2 ETL interface and perovskite absorber and introducing Cu1.8S nanocrystals to perfect the Spiro‐OMeTAD HTL is represented. A significant hysteresis‐free power conversion efficiency improvement from 18.31% to 21.64% of PSCs is achieved after modifications with the enhanced short‐circuit current density, open‐circuit voltages, and fill factor. Various advanced characterizations, including femtosecond transient absorption spectroscopy, electrochemical impedance spectroscopy, and ultraviolet photoelectron spectroscopy, elucidate that the TQD/Cu1.8S significantly contribute to the improved crystalline quality of the perovskite film with its large grain size and improved electron/holes extraction efficiencies at perovskite/ETL and perovskite/HTL interfaces. Furthermore, the long‐time ambient and light stability of PSCs are largely boosted through the TQD and/or Cu1.8S nanocrystals doping, originating from the better crystallization of perovskite, suppressing the film aggregation and crystallization of HTL, and inhibiting the ultraviolet‐induced photocatalysis of the ETL. The findings highlight the TQD and Cu1.8S can act as a superfast electrons and holes tunnel for the optoelectronic devices.
In recent years, significant advances have been achieved in the red and green perovskite quantum dot (PQD)-based light-emitting diodes (LEDs). However, the performances of the blue perovskite LEDs are still seriously lagging behind that of the green and red counterparts. Herein, we successfully developed Ni2+ ion-doped CsPbCl x Br3–x PQDs through the room-temperature supersaturated recrystallization synthetic approach. We simultaneously realized the doping of various concentrations of Ni2+ cations and modulated the Cl/Br element ratios by introducing different amounts of NiCl2 solution in the reaction medium. Using the synthetic method, not only the emission wavelength from 508 to 432 nm of Ni2+ ion-doped CsPbCl x Br3–x QDs was facially adjusted, but also the photoluminescence quantum yield (PLQY) of PQDs was greatly improved due to efficient removal of the defects of the PQDs. Thus, the blue emission at 470 nm with PLQY of 89% was achieved in 2.5% Ni2+ ion-doped CsPbCl0.99Br2.01 QDs, which increased nearly three times over that of undoped CsPbClBr2 QDs and was the highest for the CsPbX3 PQDs with blue emission, fulfilling the National Television System Committee standards. Benefiting from the highly luminous Ni2+ ion-doped PQDs, the blue-emitting LED at 470 nm was obtained, exhibiting an external quantum efficiency of 2.4% and a maximum luminance of 612 cd/m2, which surpassed the best performance reported previously for the corresponding blue-emitting PQD-based LED.
A seeded growth method to produce colloidal carbon dots (CDs) through controlling the number of seeds and reaction time, which is demonstrated to be an effective way to tune their optical properties, is developed. Color‐tunable fluorescence of CDs with blue, green, yellow, and orange emissions under UV excitation is achieved by increasing the size of the seed CDs, with the color depending on the size of the π‐conjugated domains. Strong multicolor photoluminescence of powdered samples enables realization of efficient down‐conversion white‐light‐emitting devices with correlated color temperature ranging from 9579 to 2752 K and luminous efficacy from 19 to 51 lm W−1. Moreover, color‐tunable room‐temperature phosphorescence of CD powders is demonstrated in the broad spectral range of 500–600 nm. It is related to the presence of the nitrogen‐containing groups at the surface of CDs, which form interparticle hydrogen bonds to protect the CD triplet states from quenching, and to the existence of the polyvinylpyrrolidone polymer chains at the surface of CDs. The color‐tunable room‐temperature phosphorescence from CDs demonstrated in this work exhibits potential for data encryption.
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