Optical polarization properties of TPP2MnBr4 perovskite crystal adjusted by the self-trapping state.

Low-dimensional networked organic-inorganic hybrid metal halide crystal has become an emerging hotspot material due to its opportunities and advantages in the development of white-light-emitting diodes. Therefore, its photoluminescence (PL) mechanism is important. Herein, we study the PL behavior of columniform TPP2MnBr4 crystals using multi-spectroscopy. The temperature-dependent PL data show that the PL of the TPP2MnBr4 crystal originates from the recombination of a self-trapping exciton. A polarization-dependent PL test suggests that the self-trapping exciton is anisotropic, which indicates that the distribution of self-trapping states is sensitive to the orientation of the crystal axis. Space-resolved PL spectroscopy shows that the anisotropy of PL gradually weakens along the orientation of the columniform crystal, which has a longer relaxation distance than traditional light-wave-guiding behavior. Thus, anisotropy of PL can exist before it disappears in the crystal. Our results elucidate the PL mechanism of low-dimensional networked organic-inorganic hybrid metal halide crystals and provide a foundation for advanced optical polarization devices based on them.

Activity enhancement of a photo-generated carrier in CsPbBr3 nanocrystals improved by Cd element.

Doping Cd element into perovskite materials is an effective strategy to improve the photoelectric property. However, the further discussion for carrier dynamic behavior in perovskites affected by Cd element remains not sufficient. In this research letter, based on steady and transient spectroscopy, it is found that adding Cd element into CsPbBr3 nanocrystals can enhance the activity of photo-generated carriers and accompany with the optimization of crystal structure. The former improves the carrier heating effect, which makes carrier keep high temperature for a long time and accelerate the bimolecular and the Auger recombination simultaneously. The latter can restrict the monomolecular recombination through passivating the defect states. Finally, they together improve the photoluminescence characteristics of the Cd doped CsPbBr3 nanocrystals and make them exhibit a huge potential in the fields of optoelectronics or photo-catalysis.

Cooling and diffusion characteristics of a hot carrier in the monolayer WS2.

The characteristics of a hot carrier distributed in the C excitonic state of the monolayer WS2 is investigated by exploiting the transient absorption (TA) spectroscopy. The hot carrier cooling lifetime gradually prolongs from 0.58 ps to 2.68 ps with the absorbed photon flux owing to the hot phonon bottleneck effect, as the excitation photon energy is 2.03 eV. Meanwhile, the normalized TA spectra shows that the spectral feature of hot carriers is different from that of normal carriers. Based on the modified Lennard-Jones model, the average distance among hot carriers can be estimated according to the peak shift of TA spectra and the diffusion velocity can also be calculated simultaneously. The hot carrier limits the diffusion of the photo-generated carrier at the initial several picoseconds. These results help people to elucidate the hot carrier dynamics in 2D TMDCs and give guidance on the designing and optimizing the TMDC-based electronic devices of high performance.

Exploring the emission mechanism of dichromatic white-light quantum-dot light-emitting diodes using wavelength-resolved transient electroluminescence analysis.

Exploring electroluminescence (EL) processes is extremely vital to fabricate efficient white-light quantum-dot light-emitting diodes (QLEDs). A model white QLED consisting of a bilayer CdSe/ZnSeS quantum-dot (QD)//CuInS2/ZnS QDs emissive layer has been used to analyze the white-light emission mechanism. In this design, the CdSe/ZnSeS QDs and CuInS2/ZnS QDs contribute to the blue and yellow emissions, respectively, in the dichromatic white QLED. Wavelength-resolved transient EL (TrEL) results demonstrate that the excitons are mainly formed on the CuInS2/ZnS QDs in the QLED operated at low biases due to the low barrier to hole injection and energy transfer from the CdSe/ZnSeS QDs to the CuInS2/ZnS QDs. Further, the TrEL decays of both white and monochromic devices reveal that the emission behavior of the white QLED is closely related to that of the monochromic device, but is minimally affected by the interactions between different emission units. The simulation results performed by the solar cell capacitance simulator model agree well with the experimental data. Our results show an insight into the EL processes in the white device QLED and demonstrate a powerful tool to investigate emission behavior of the white QLEDs.

Solvent-dependent ultrafast optical response of conjugated push-pull chromophores.

Two new difluoroboron ß-carbonyl cyclic ketonate complexes C2B and DC2B were investigated using several spectroscopic methods. Relative to the absorption spectra, the fluorescence spectra were more affected by the polarity of the solvent. Also, compound C2B showed a more pronounced Stokes' shift after solvent polarity increased. Transient absorption measurements then demonstrated the relaxation behaviour of the excited state compound molecule. The kinetic results showed that the excited state C2B in tetrahydrofuran (THF) can return from the intramolecular charge-transfer (ICT) state and the initial excited state to the ground state. The kinetic relaxation pathway after THF was replaced by dimethyl sulfoxide became single. When the carbazole unit was introduced, DC2B also exhibited an ICT state but there was no significant difference in the excited state relaxation path after solvent polarity was changed. The results indicated that C2B is more susceptible to solvent polarity regulation. The global fit results revealed that an increase in the solvent polarity prolonged the lifetime of the ICT state of compound C2B and had the opposite effect on compound DC2B. These results provide guidance for understanding the relationship between solvent polarity and the designing and synthesizing advanced compound materials.

Emitting color tunable carbon dots by adjusting solvent towards light-emitting devices.

Carbon dots (CDs), one of the most significant classes of carbon-based nanophosphors, have attracted extensive attention in recent years. However, few attempts have been reported for realizing CDs with tunable emissions, especially for obtaining the red-light emissions with high photoluminescence quantum yields. Herein, we synthesized CDs with different chromatic blue, green and red emissions by facilely changing the reaction solvent during hydrothermal conditions. The photoluminescence quantum yields of 34%, 19% and 47% for the blue, green and red emissions, respectively, were achieved. Furthermore, the solid-state CD/PVA composite films were constructed through mixing the CDs with PVA polymer, in which the self-quenching of photoluminescence of CDs had been successfully avoided benefiting from the formation of hydrogen bonds between the CDs and PVA molecules. Finally, the warm white light emitting diode (WLED) was fabricated by integrating CD/PVA film on a UV-LED chip. The WLED exhibited the Commission International de l'Eclairage coordinates (CIE) of (0.38, 0.34), correlated color temperature of 3913 K and color rendering index of 91, respectively, which were comparable with the commercial WLEDs.

Modulation of the photoluminescence in carbon dots through surface modification: from mechanism to white light-emitting diodes.

Carbon dots (CDs) have emerged as a new type of fluorescent material because of their unique optical advantages, such as high photoluminescence quantum yields (QYs), excellent photo-stability, excitation-dependent emissions, and low toxicity. However, the photoluminescence mechanism for CDs remains unclear, which limits their further practical application. Here, CDs were synthesized via a solvothermal route from citric acid and urea. Through the oxidation and reduction treatment of pristine CDs, the origin of the photoluminescence and the involved mechanism were revealed. We found that the blue/green/red emissions originated from three diverse emitting states, i.e. the intrinsic state, and C=O- and C=N-related surface states, respectively. Based on the as-prepared CDs, a pH sensor depending on the radiometric luminescence detection was developed. Furthermore, we constructed CD/PVP (PVP, polyvinylpyrrolidone) composite films, which exhibited white light emission with photoluminescence QYs of 15.3%. The white light emission with different correlated color temperatures (CCTs), from 4807 K to 3319 K, was obtained by simply changing the amount of PVP solution. Benefiting from the white light-emitting solid-state films, single-component white light-emitting diodes were fabricated with an average color rendering index value (Ra) of 80.0, luminous efficiency of 10.2 lm W-1, and good working stability, thus indicating a promising potential for practical lighting applications.

Spontaneous emission of semiconductor quantum dots in inverse opal SiO2 photonic crystals at different temperatures.

The photoluminescence (PL) characteristics of CdSe quantum dots (QDs) infiltrated into inverse opal SiO2 photonic crystals (PCs) are systemically studied. The special porous structure of inverse opal PCs enhanced the thermal exchange rate between the CdSe QDs and their surrounding environment. Finally, inverse opal SiO2 PCs suppressed the nonlinear PL enhancement of CdSe QDs in PCs excited by a continuum laser and effectively modulated the PL characteristics of CdSe QDs in PCs at high temperatures in comparison with that of CdSe QDs out of PCs. The final results are of benefit in further understanding the role of inverse opal PCs on the PL characteristics of QDs.

Colloidal PbSe quantum dot-solution-filled liquid-core optical fiber for 1.55 µm telecommunication wavelengths.

We have studied the optical properties of PbSe colloidal quantum dot-solution filled hollow core multimode silica waveguides as a function of quantum dot-solution concentration, waveguide length, optical pump power and choice of organic solvent in order to establish the conditions to maximize near infrared spontaneous emission intensities. The optical performance was compared and showed good agreement with a simple three level system model for the quantum dots confined in an optical waveguide. Near infrared absorption-free solvent of tetrachlorethylene was confirmed to be a good candidate for the waveguide medium due to the enhancement of output intensity from the liquid-core fiber compared to the performance in toluene-based fiber. This approach demonstrates a useful method for early characterization of quantum dot materials in a waveguide test-bed with minimal material processing on the colloidal nanoparticles.

High-Performance Tandem Quantum-Dot Light-Emitting Diodes Based on Bulk-Heterojunction-Like Charge-Generation Layers.

In this study, the fundamental but previously overlooked factors of charge generation efficiency and light extraction efficiency (LEE) are explored and collaboratively optimized in tandem quantum-dot light-emitting diodes (QLEDs). By spontaneously forming a microstructured interface, a bulk-heterojunction-like charge-generation layer composed of a poly(3,4-ethylenedioxythiophene):poly(styrene sulfonate)/ZnO bilayer is fabricated and an ideal charge-generation efficiency surpassing 115% is obtained. The coupling strength of the waveguide mode for the top unit and the plasmon polariton loss for the bottom unit are highly suppressed using precise thickness control, which increases the LEE of the tandem devices. The red tandem QLED achieves an exceptionally low turn-on voltage for electroluminescence at 4.0 V and outstanding peak external quantum efficiency of 42.9%. The ultralow turn-on voltage originates from the sequential electroluminescence turn-on of the two emissive units of the tandem QLED. Benefiting from its unique electroluminescent features, an easily fabricated optical-electrical dual anti-counterfeiting display is built by combining a dichromatic tandem QLED with masking technology.

Competition of Carrier Kinetics Contributes to Amplified Spontaneous Emission in Quasi-2D/3D (PBA)2MAn-1PbnBr3n+1 Thin Films under Strip Light Mode.

Quasi-2D halide perovskites have potential in lasing due to their amplified spontaneous emission (ASE) properties. The ASE of (PBA)2MAn-1PbnBr3n+1 thin films has been confirmed by photoluminescence (PL) testing using stripe light excitation (SLE). The ASE threshold decreases with decreasing environmental temperature (TE) or increasing number of inorganic layers (n). Using the transient absorption technique, the Auger recombination and the cooling process of the high-activity carrier are accelerated with the decrease of n or TE. A new ASE mechanism is proposed where high-activity carriers directly emit photons under photon perturbation from adjacent sites, leading to the accumulation and amplification of emitted photons only in the SLE region for ASE to occur. In addition, the reduction of n promotes light scattering between nano-thin layers, which supports a rapid increase in the ASE signal after the ASE threshold is crossed.

Inhibited local thermal effect in upconversion luminescence of YVO4:Yb³âº, Er³âº inverse opals.

Upconversion Luminescence (UCL) of YVO4:Yb³âº, Er³âº inverse opal photonic crystals (IOPCs) was investigated in contrast to the references under the excitation of a 980-nm laser diode. Besides the traditional modification on UCL and dynamics, it is significant to observe that in the IOPCs the temperature quenching and local thermal effect was greatly suppressed.

Electronic and Excitonic Processes in Quantum Dot Light-Emitting Diodes.

A modified Langevin model has been proposed to study the electronic and excitonic dynamic processes in quantum dot light-emitting diodes (QLEDs), and the electroluminescence onset processes of the QLEDs under different charge-injection conditions have been explored. The simulation results are in good agreement with experimental curves, confirming the feasibility of this model. It is demonstrated that the formation of an exciton on the quantum dots (QDs) with one electron injected first followed by one hole is much more effective than that with the reverse sequence. That is, charging a QD with one electron first is more favorable for device performance enhancement, which is attributed to the low (high) Auger recombination rate of negative (positive) trions of commonly used type I QDs. Additionally, we demonstrate that enough electron injection is one of the prerequisites for high-performance QLEDs based on these type I QDs.

Calibrating the Hole Mobility Measurements Implemented by Transient Electroluminescence Technology.

To date, measuring the carrier mobility in semiconductor films, especially for the amorphous organic small-molecule films, is still a big challenge. Here, we demonstrate that transient electroluminescence (TrEL) spectroscopy with quantum-dot light-emitting diodes as the platform is a feasible and reliable method to evaluate the carrier mobility of such amorphous films. The position of the exciton formation zone is precisely determined and controlled by employing a quantum dot monolayer as the emissive layer. The electrical field intensity across the organic layer is evaluated through the charge density at the electrode calculated by the transient current. Then, the charge carrier mobility is obtained by combining the electroluminescence (EL) delay time and the thickness of the organic layer. Additionally, we demonstrate that the large roughness of the organic layer leads to serious charge accumulation and, hence, a high localized electrical field, which provides preferred charge injection paths, reducing the EL delay time and underestimating the EL delay time. Therefore, a thick organic film is the prerequisite for a reliable measurement of charge carrier mobility, which can circumvent the negative effect of film roughness.

Synthesis of star-shaped monodisperse oligo(9,9-di-n-octylfluorene-2,7-vinylene)s functionalized truxenes with two-photon absorption properties.

A series of new star-shaped monodisperse conjugated truxene derivatives bearing oligo(fluorene-vinylene) arms (Tr-OFVn, n = 1, 2, 3, 4) have been synthesized. It is found that the conjugation of the oligomers can be extended with prolonging the arms. Notably, the branched oligomers Tr-OFVn without strong donor and acceptor units exhibit two-photon absorption properties, and the two-photon absorption cross sections (δ(max)) increase with increasing the number of fluorene-vinylene units in the arms. The maximum value of δ(max) reaches 8073 GM for compound Tr-OFV4, which made it one of the most competitive compounds with enhanced TPA cross section. It provides a new platform for exploiting strong TPA compounds, in which the extended π-conjugated systems are involved in the absence of strong donor and acceptor units.

[Low driving voltage in organic light-emitting diodes with NPB/MoO3/NPB as a hole transport layer].

Driving voltage of organic light-emitting diodes (OLEDs) was lowered by applying (NPB/MoO3)(x)/NPB as a hole transport layer (HTL). (NPB/MoO3)(x) was multi-layer periodic (MLP) structure with x changed from 0 to 3. Compared with the conventional device with 0-periodic structure, the driving voltage of the device with 1-periodic structure was the lowest. This was due to charge transfer (CT) complex formation between NPB and MoO3. The driving voltage of tris (8-hydroxyquinoline) aluminum (Alq3)-based organic light-emitting devices (OLEDs) could be lowered by 0. 8 V at 1 000 cd x m(-2) by using multiple structure of NPB/MoO3/NPB.

Investigation of Hot Carrier Cooling Dynamics in Monolayer MoS2.

The hot carrier cooling dynamics in the C-excitonic state of monolayer MoS2 is slowed down by the hot phonon bottleneck and Auger heating effects, as exploited by ultrafast transient absorption spectroscopy. The hot carrier cooling process, determined by the hot phonon bottleneck, can be prolonged through rising the excitation photon energy or increasing the absorbed photon flux. By inducing the Auger heating effect under higher absorbed photon flux, the hot carrier lifetime also increases at the low excitation photon energy. When these two effects are combined under higher excitation photon energy and higher absorbed photon flux, the hot phonon bottleneck is gradually weakened because of Auger recombination. In addition, the similar hot carrier phenomenon can be observed in A/B excitonic states owing to the same physical mechanism. Our work establishes a solid photophysics foundation for 2D transition-metal dichalcogenide applications in advanced energy conversion, optical quantum communication, quantum technology, etc.

Near-unity blue-orange dual-emitting Mn-doped perovskite nanocrystals with metal alloying for efficient white light-emitting diodes.

The tunable dual-color emitting Mn2+ doped CsPbCl3-xBrx nanocrystals (NCs) with near-unity photoluminescence quantum yield (PL QY) were synthesized through post-treatment of metal bromide at room temperature for fabrication of efficient warm white light-emitting diodes (WLEDs). Especially, the CdBr2 treated blue-orange emitting Mn doped NCs with various Mn/Pb molar feed ratios exhibit higher PL QY of 97% and longer Mn2+ PL lifetime of 0.9 ms. It is surprisingly found that the X-ray diffraction peak at 31.9° is almost not changed with increasing Br composition, meaning formation of metal alloying due to incorporation of amount of divalent cation in NCs. The strong and stable Mn2+ PL at temperature ranging from 80 K to 360 K are revealed and the temperature-dependent energy transfer efficiencies in Mn2+ doped CsPbCl1.5Br1.5 NCs are obtained. The enhancement mechanism of Mn2+ PL QY was attributed to improved energy transfer from exciton to Mn2+ d-d transition and suppressed defect state density after post-treatment. The efficient warm WLEDs with color rendering index of 90 and luminous efficacy of 92 lm/W at 10 mA were fabricated by combining blue-orange dual-emitting Mn2+ doped CsPbCl3-xBrx@SiO2 and green emissive CsPbBr3@SiO2 NCs with violet GaN chips.

Study of the Photoluminescence Characteristics of 4,4'-((1E,1'E)-Quinoxaline-2,3-diylbis(ethene-2,1-diyl))bis(N,N-dimethylaniline).

A comparative investigation on the photophysical properties of a quinoxaline derivative 4,4'-((1E,1'E)-quinoxaline-2,3-diylbis(ethene-2,1-diyl))bis(N,N-dimethylaniline) (QDMA2) was performed by employing many spectroscopies. Based on the pump-dump/push-probe measurement, it is found that a solvent-stabilized charge-transfer state can participate in the relaxation of excited QDMA2 with increasing solvent polarity. Meanwhile, the aggregated QDMA2 molecules were engineered into the organic light-emitting diode test, which showed a correlated color temperature value of 1875 K. With the help of a diamond anvil cell, the pressure-dependent photoluminescence of aggregated QDMA2 shows that the intermolecular interaction can affect the color and intensity of photoluminescence through adjusting the band gap and irradiative channel of the aggregated molecules. These results are important for understanding the structure-property relationships and the rational design of functional materials for optoelectronic applications.

Efficient Structure for InP/ZnS-Based Electroluminescence Device by Embedding the Emitters in the Electron-Dominating Interface.

The charge-carrier distribution has been an important parameter in determining the efficiency of quantum-dot-based light-emitting diodes (QLEDs). In this Letter, we demonstrate a new inverted device structure of ITO/ZnO/polyethylenimine/quantum dots (QDs)/1,3,5-tris(N-phenylbenzimidazole-2-yl)benzene (TPBi)/4,4'-bis(9-carbazolyl)-2,2'-biphenyl (CBP)/MoO3/Al for improving the efficiency of InP-QD-based QLEDs. By introducing a thin layer of electron transport materials, the hole accumulation at the hole transport layer and the QD interface is largely reduced, which suppresses the quenching effect of holes on the QD emission. Compared with the conventional device structure with the emitters at ZnO/CBP pn junction, the peak current efficiency (external quantum efficiency) increases from 3.83 (5.17 cd/A) to 6.32% (8.54 cd/A) by imbedding the QDs at the electron-dominating interface of ZnO/TPBi. The analysis reveals that an internal quantum efficiency of nearly 100% is achieved for the InP-QD-based device (with a photoluminescence quantum yield of 32%). This work provides an alternative device structure for achieving high-efficiency QLED devices.