摘要:We designed and synthesized two novel thermally activated delayed fluorescence emitters, 3-CzAIAd and 3-DPFCzAIAd, and performed a comparative analysis with their isomeric counterparts, 4-CzAIAd and 4-DPFCz-AIAd. The substitution position of the carbazole unit plays a critical role in modulating the photophysical properties of the emitters and the device performance of organic light-emitting diodes. Emitters with carbazole units substituted at the 3-position of phthalimide group exhibited higher triplet energy levels, smaller singlet-triplet energy gaps, lower photoluminescence quantum yields, and more red-shifted emission spectra. Devices incorporating 3-DPFCzAIAd achieved a maximum external quantum efficiency of 20.8%, a peak current efficiency of 57.1 cd·A⁻¹, and an operational half-lifetime of 260 h under an initial luminescence of 500 cd·m⁻². Conversely, while devices based on 4-DPFCzAIAd exhibited a higher peak EQE of 28.2%, they experienced a shorter operational lifetime of 178 h under an initial luminescence of 500 cd·m⁻² and more pronounced efficiency roll-off of up to 77%.
摘要:Photoluminescent aerogels, possessing the combined features of aerogels and luminescent materials, are a novel type of porous luminescent materials. Photoluminescent aerogels are characterized by unique properties, such as large specific surface area, high porosity, flexible structure, and controllable optical properties, and thus hold wide promise for diverse applications, particularly in sensing and optoelectronic devices. Focusing on photoluminescent aerogels, this review summarizes the preparation methods of aerogels, systematically introduces the aerogel according to the classification of luminescent centers, and discusses the application of the aerogel in the fields of sensing and optoelectronic devices. Finally, challenges and perspectives of photoluminescent aerogels are discussed.
摘要:Over recent years, research into the upconversion luminescence properties of highly doped Er3+ nanocrystals has undergone rapid advancement. Compared to traditional doping materials, these materials exhibit unique features such as multi-band excitation, strong excitation wavelength penetration, dynamic control over optical color, and highly sensitive to external field stimuli, showing great promise in various research domains including optical information security, temperature sensing, and bioimaging. This review provides a comprehensive overview of the techniques for tuning upconversion luminescence intensity, emission colors, decay characteristics, and excitation bands through ways of such as matrix composition, structural design, and energy transfer processes. Additionally, we explore the impact of external field stimuli such as temperature, pressure, and metal surface electric fields on the luminescence properties of highly Er3+ doped nanocrystals. The mechanisms behind luminescence enhancement are discussed in terms of increased multiphoton transition probabilities and reduced non-radiative energy losses. Finally, we summarize the research on modulating excitation modes in highly doped Er3+ nanocrystals and propose directions for future investigations.
摘要:Near-infrared (NIR) phosphor-converted light-emitting diodes (pc-LEDs) hold great promise for versatile applications such as non-destructive analysis, machine vision and biological imaging. Currently, exploring efficient broadband tunable NIR-Ⅰ-emitting phosphors applicable for NIR pc-LEDs has been an ongoing focus among material researchers. Herein, we firstly synthesize two kinds of NIR-emitting perovskite-type Sr3MgTa2O9∶Cr3+ and Ba3MgTa2O9∶Cr3+ phosphors via the solid-state reaction, both of which possess the characteristic of broadband emission bands covering the NIR-Ⅰ spectral range from 700 nm to 1 000 nm. Fine regulating Ba2+/Sr2+ dopant ratio in (Sr1-mBam)3MgTa2O9∶Cr3+ solid-solution phosphors further achieves the continuously adjustable NIR luminescence with the emission peak position tuning from 786 nm to 848 nm, due to the weakened crystal field environment of crystallographic Mg2+ site which is occupied by Cr3+ ion. The representative Sr0.4Ba0.6MgTa2O9∶0.015Cr3+ phosphor exhibits high internal quantum efficiency (82.1%) and favorable thermal stability (I423 K/I298 K=73.6%), which is competitive with some other emerging Cr3+-doped NIR-emitting phosphors. Finally, a prototype NIR pc-LED by utilizing Sr0.4Ba0.6MgTa2O9∶0.015Cr3+ phosphor and a blue LED chip achieves the ideal NIR output with satisfactory luminous efficacy of 63.28 lm/W, exhibiting its enormous potential for practical applications in the fields of veins imaging and night vision. The present study develops a series of novel NIR-emitting perovskite-type phosphors with excellent luminescent properties based on the mineral-type structural prototype and cationic substitution strategy, which will provide a basis for design of Cr3+-doped broadband tunable NIR-Ⅰ-emitting phosphors.
摘要:Red emitting phosphors with high thermal stability are of great significance for improving the performance of phosphor-converted WLEDs(pc-WLEDs). Introducing sensitizers to transfer energy to the luminescent center and improve the thermal stability of phosphor is an effective strategy for developing high-performance WLEDs. Here, a double perovskite structure compound Gd2ZnTiO6 is selected as the host to produce series of Sm3+, Eu3+ activated red phosphors, and the energy transfer process from Sm3+ to Eu3+ is discussed in detail. This work confirms the positive effect of energy transfer on the thermal stability of the single Eu3+-activated phosphor. The PL intensity of the co-dopping samples at 150 ℃ remains 74% of that at room temperature. This result provides a practical evidence for the theory that energy transfer from sensitizer to activators can effectively suppress the thermal quenching of phosphors.
“In the field of high-energy X-ray imaging, (Gd, Lu)2O3:Eu scintillation ceramics have shown promising applications. Researchers have prepared Eu0.1Gd0.6Lu1.3O3 nano-powders and ceramics, investigating the impact of pre-sintering temperature on microstructure, optical, and luminescence properties. The ceramics pre-sintered at 1,625°C for 2 hours and post-treated with HIP at 1,750°C for 3 hours in argon exhibit the highest in-line transmittance of 75.2% at 611 nm. The PL, PLE, and XEL intensities of the HIP post-treated ceramics show a trend of first ascending and then descending with the increase of pre-sintering temperature.”
摘要:(Gd,Lu)2O3∶Eu scintillation ceramics have promising applications in the high-energy X-ray imaging. Eu0.1Gd0.6Lu1.3O3 nano-powders with pure phase were prepared from the precursor calcined at 1 050 ℃ for 4 h by the co-precipitation method. Using the synthesized nano-powders as initial material, Eu0.1Gd0.6Lu1.3O3 ceramics were fabricated by vacuum pre-sintering at different temperatures for 2 h and hot isostatic pressing (HIP) at 1 750 ℃ for 3 h in argon. The influence of pre-sintering temperature on the microstructure, optical and luminescence properties was investigated. The Eu0.1Gd0.6Lu1.3O3 ceramics pre-sintered at 1 625 ℃ for 2 h combined with HIP post-treatment show the highest in-line transmittance of 75.2% at 611 nm. The photoluminescence (PL) and X-ray excited luminescence (XEL) spectra of the Eu0.1Gd0.6Lu1.3O3 transparent ceramics demonstrate a strong red emission peak at 611 nm due to the 5D0→7F2 transition of Eu3+. The PL, PLE and XEL intensities of the HIP post-treated Eu0.1Gd0.6Lu1.3O3 ceramics show a trend of first ascending and then descending with the increase of pre-sintering temperature. The thermally stimulated luminescence (TSL) curve of the HIP post-treated Eu0.1Gd0.6Lu1.3O3 ceramics presents one high peak at 178 K and two peaks with lower intensities at 253 K and 320 K. The peak at 320 K may be related to oxygen vacancies, and the luminescence peak at 178 K is related to defects caused by the valence state changes of Eu3+ ions.
摘要:Ba5SiO4Cl6∶Eu2+,Ln3+ blue long-persistent phosphors were synthesized by high-temperature solid-state method and their structure and luminescence properties were characterized by means of X-ray diffraction, excitation and emission spectroscopy, afterglow decay curves, afterglow spectroscopy and thermoluminescence. The results showed that under the excitation of UV light at 347 nm, both Eu2+ single-doped and Eu2+, Ln3+ co-doped phosphors emit bright blue light, and the emission spectra showed that they have two obvious peaks located at 440 nm and 500 nm, which belong to the characteristic emission of Eu2+ at different lattice positions (4f 65d1-4f 7). The incorporation of Ln3+ introduced hybrid energy levels within the bandgap, resulting in traps of varying depths, which enhanced the afterglow performance of the material to different extents. Among them, the Ba5SiO4Cl6∶Eu2+, Ho3+ samples showed the best performance with an afterglow time of more than 12 h. The Ba5SiO4Cl6∶Eu2+,Er3+ samples showed a 12-fold increase in the initial brightness compared to the singly doped samples. The doping of Dy3+ effectively increased the concentration of the deep traps (T2) in the sample, which was expected to be used for optical data storage.
摘要:Ce3+ doped Ba3Y2(BO3)4 phosphors were synthesized by the solid-state reaction technique. The crystal structure was analyzed by the X-ray diffraction patterns. The photoluminescence excitation and emission spectra, photoluminescence decay curves, the CIE coordinates and temperature dependent emission spectra were studied. The bright blue emission of Ba3Y2(BO3)4∶Ce3+ phosphors peaks around 420 nm was observed under the UV excitation, the full width at half maximum is over 83 nm. The integrated luminescence intensities increase first and then decrease with increasing Ce3+ concentration. The CIE coordinates of the samples with the increasing of Ce3+ concentration change slightly, indicating that the color stability of the samples was excellent. With the temperature increasing the emission intensity of samples decreased, the thermal stability of the sample needs to be improved. A white LED was fabricated by using a 365 nm LED chip combined with Ba3Y2(BO3)4∶Ce3+ phosphor and commercial phosphor, the CIE was (0.33, 0.39), CCT was 5 570 K, and Ra was 92.6. These results indicated that Ba3Y2(BO3)4∶Ce3+ phosphor could be as a blue broad emission band LED phosphor.
摘要:A series of YbNbO4 phosphors doped with x% (ion concentration) Ho3+ (x=1, 2, 5, 10, 15) were prepared by high temperature solid phase method. The synthesized sample was characterized by X-ray diffraction (XRD) and Fourier transform infrared spectroscopy (FT-IR), and the results showed that the synthesized fluorescent powder sample had a monoclinic phase structure with a space group of I2/a. At the same time, the electronic structure (band and density of states) of the YbNbO4 matrix was calculated. YbNbO4 has a direct band gap with a bandgap width of 4.223 eV. Further investigation was conducted on the effect of Ho3+ ions doping concentration on emission spectra, and it was screened that a 2% Ho3+ ions doping concentration had the best luminescence effect. In addition, samples doped with 2% Ho3+ were excited at different powers. By fitting the emission peak to the excitation light power, it was further concluded that the upconversion of Ho3+ ions to red light at 666 nm (5F5→5I8) and green light at 543 nm (5S2/5F4→5I8) emission both belong to two-photon processes. In addition, based on the fluorescence intensity ratio (LIR) technique, the temperature dependent spectra of 2% Ho3+ doped samples were measured in the temperature range of 300-570 K, and the absolute sensitivity (Sa) and relative sensitivity (Sr) used to characterize the optical temperature sensing performance were calculated. The results showed that the Sr of the samples reached a maximum value of 0.36%·K-1 at 420 K.
关键词:upconversion luminescence;high temperature solid phase method;fluorescence intensity ratio;first principles calculation
摘要:To investigate the effect of GaAs insertion layer on the luminescence performance of 905 nm wavelength InGaAs multi quantum well materials, based on InGaAs/InAlGaAs and InGaAs/AlGaAs quantum well materials, four period 905 nm wavelength InGaAs multi quantum wells were grown using metal organic compound chemical vapor deposition (MOCVD) technology. Atomic force microscopy (AFM) and X-ray diffraction (XRD) analyses revealed that the GaAs insertion layer optimizes the surface roughness and crystal quality of both materials. Room temperature photoluminescence (PL) testing further demonstrated that the GaAs insertion layer improves the energy band structure of the materials, thereby improving luminescence efficiency. Variable temperature and variable power PL tests show that for InGaAs/InAlGaAs materials, after the GaAs insertion layer is introduced, the wavelength changes in an “S” shape with increasing temperature, and the characteristic value is less than 1.The radiation recombination mechanism at low temperature changes from free exciton recombination to “localized states” luminescence. In contrast, for InGaAs/AlGaAs materials, the GaAs insertion layer does not alter the radiation recombination mechanism. This article is significant for advancing the understanding of the effects of the GaAs insertion layer on the optical properties and carrier recombination mechanisms of InGaAs/InAlGaAs and InGaAs/AlGaAs multiple quantum well materials.
“In the field of 2D transition metal dichalcogenides, researchers have reported a photoluminescence enhancement effect of 1L WS2 at room temperature when constructing it into 1L-WS2/hBN/1L-MoS2 vertical heterostructures. The photoluminescence enhancement factors can be up to 4.2, which provides a feasible way to optimize the performance of TMD-based optoelectronic devices.”
摘要:Two-dimensional(2D) transition metal dichalcogenides(TMDs) and their heterostructures(HSs) exhibit unique optical properties and show great promise for developing next-generation optoelectronics. However, the photoluminescence(PL) quantum yield of monolayer(1L) TMDs is still quite low at room temperature, which severely limits their practical applications. Here we report a PL enhancement effect of 1L WS2 at room temperature when constructing it into 1L-WS2/hBN/1L-MoS2 vertical HSs. The PL enhancement factors(EFs) can be up to 4.2. By using transient absorption(TA) spectroscopy, we demonstrate that the PL enhancement effect is due to energy transfer from 1L MoS2 to 1L WS2. The energy transfer process occurs on a picosecond timescale and lasts more than one hundred picoseconds which indicates a prominent contribution from exciton-exciton annihilation. Furthermore, the PL enhancement effect of 1L WS2 can be observed in 2L-MoS2/hBN/1L-WS2 and 3L-MoS2/hBN/1L-WS2 HSs. Our study provides a comprehensive understanding of the energy transfer process in the PL enhancement of 2D TMDs and a feasible way to optimize the performance of TMD-based optoelectronic devices.
关键词:transition metal dichalcogenide;van der Waals heterostructures;photoluminescence;Förster resonance energy transfer;exciton-exciton annihilation
摘要:This work shows that the carbonyl oxygen in the solvent N-ethyl-2-pyrrolidone(NEP) has a stronger electronegativity than N-methyl-2-pyrrolidone(NMP) by extended huckel theoretical calculations, and predicts a stronger interaction between NEP and PbI2. The study employs a solvent-regulation-assisted crystallization strategy to effectively suppress the formation of solvent-perovskite complex intermediates, improving the crystallization quality of the perovskite films. The highest power conversion efficiency(PCE) of FAPbI3 perovskite solar cells fabricated in atmosphere increased from 20.25% to 21.05%, and the average efficiency improved from 18.43% to 19.50%. The stability of unencapsulated devices was maintained at 82.1% of their initial efficiency after 1 200 h under 10%-20% RH at room temperature. Moreover, this strategy is applicable to other perovskite chemical compositions(FA0.95Cs0.05PbI3) for perovskite precursor solutions, demonstrating the universality of which. This research would contribute to the research on the ambient preparation of perovskite solar cells.
关键词:perovskite solar cells;ambient printed devices;crystallization regulation
摘要:High-performance InGaN-based red LEDs are urgently required for Micro LED displays based on Ⅲ-nitride materials. In this work, we use polarization engineering to construct a nitrogen-polar (N-polar) InGaN-based red LED with a compositionally graded InGaN layer as the last quantum barrier (LQB) layer. The numerical simulation results show that the opposite polarization electric field in N-polar nitride materials effectively enhances the confinement of carriers in the quantum well and reduces the turn-on voltage of device. Importantly, the interface between the compositionally graded InGaN LQB and p-GaN simultaneously forms electron and hole potential wells, enabling efficient radiative recombination and thus significantly improving the luminous performance of InGaN-based red LEDs. This work provides a new approach for the design and fabrication of efficient InGaN-based red LEDs.
摘要:Based on the advantages of high color purity, multi-resonance thermally activated delayed fluorescence (MR-TADF) materials have attracted significant attention for their potential value in high-precision displays. This work took 12,12-dimethyl-4H-benzo[9,1]quinolino[3,4,5,6,7-defg]acridine-4,8(12H)-dione (DQAO) as the core skeleton, introducing sidechain groups with different electronic properties and performing virtual screening and fluorescence performance evaluation on molecular structures. A set of potential molecules with both narrow bands and deep blue emission were designed, and strategy for high-performance luminescent materials based on N/CO was proposed. This study comprehensively evaluated the emission characteristics such as triplet-singlet energy splitting (ΔEST), oscillator strength, and wavelength of over 70 candidates via quantum chemical methods. It was found that electron acceptors substituted at the N-position are conducive to enhancing oscillator strength and reducing reorganization energy (Eλ), which estimates the full width at half maxima (FWHM) of the emission, while electron donors tend to reduce the ΔEST. The results of this study indicate that regulating the electronic properties of N-position substituents will significantly reduce the ΔEST of MR-TADF molecules, effectively enhance their oscillator strength, and achieve the desired emission wavelength, thereby realizing high-performance narrow-band emission characteristics. This study not only provides new molecular design ideas and effective structural data sets for the efficient design of MR-TADF molecules but also lays the theoretical foundation for further optimizing the performance of fluorescent materials based on the advantages of the N-position and the electronic properties of modifying groups.
关键词:full width at half maxima;donor-acceptor;reorganization energy;virtual screening
摘要:Carbon dots are a new type of zero-dimensional carbon-based nanomaterials with many advantages, such as small size, low toxicity and easy surface functionalization. The emergence of carbon dots provides new ideas for targeted delivery of drugs to achieve cancer therapy. This review systematically describes the progress of the application of carbon dots as carriers for drug delivery. Firstly, the classification and synthesis methods of carbon dots are described. Secondly, the research progress of different kinds of drug delivery (chemotherapeutic drugs, photosensitizers, photothermal agents, etc.) based on carbon dots at home and abroad in recent years is summarized. Finally, the challenges and the application prospects are discussed, which is intended to provide some ideas for the researchers who are engaged in the research of carbon dots in the field of drug delivery.
摘要:Bisulfite (HSO3-) as an important food additive, is widely used in daily life. But excessive use and abuse can cause harmful effects on organisms and the environment. Concurrently, HSO3- as a derivative of the signaling molecule (SO2) in the body, plays a huge role in normal physiological activities. But the abnormal expression and excessive intake of HSO3- in the body can lead to a number of diseases. Therefore, it is of great significance to detect and monitor HSO3- in vivo and in the environment with the specificity and sensitivity. Herein, a near-infrared HSO3- fluorescent probe (CL) with D-π-A structure was synthesized by condensation reaction using N-ethylcarbazole as electron donor group and 2-oxo-4-phenyl-2,5-dihydro3-furanonitrile as electron acceptor group. The near-infrared fluorescence was declined and the wavelength was blue-shifted after the probe CL recognizes HSO3-. The nucleophilic addition sensing mechanism of probe CL to HSO3- was verified by high resolution mass spectrometry (HR-MS) and theoretical calculation. The probe CL has the advantages of near-infrared emission (λem=685 nm), large Stokes shift (195 nm), high selectivity and sensitivity (49 nmol/L). In addition, probe CL has been prepared into a test paper and the on-site and rapid detection of HSO3- in water samples is realized by connection with smartphones. Most importantly, the probe has been successfully applied to fluorescence imaging of HSO3- in living mice.
关键词:bisulfite;near-infrared fluorescent probe;carbazole derivative;environmental water samples;bioimaging