日本物理学会誌及びJournal of the Physical Society of Japanの月刊について

: The unpolarized absorption and circular dichroism spectra of the fundamental vibrational transitions of the chiral molecule, 4-methyl-2-oxetanone, are calculated ab initio. Harmonic force fields are obtained using Density Functional Theory (DFT), MP2, and SCF methodologies and a 5S4P2D/3S2P (TZ2P) basis set. DFT calculations use the Local Spin Density Approximation (LSDA), BLYP, and Becke3LYP (B3LYP) density functionals. Mid-IR spectra predicted using LSDA, BLYP, and B3LYP force fields are of significantly different quality, the B3LYP force field yielding spectra in clearly superior, and overall excellent, agreement with experiment. The MP2 force field yields spectra in slightly worse agreement with experiment than the B3LYP force field. The SCF force field yields spectra in poor agreement with experiment.The basis set dependence of B3LYP force fields is also explored: the 6-31G* and TZ2P basis sets give very similar results while the 3-21G basis set yields spectra in substantially worse agreements with experiment. jg

Ab initio calculation of vibrational absorption and circular dichroism spectra using density functional force fields

Quantum dot (QD) light-emitting diodes (LEDs) are ideal for large-panel displays because of their excellent efficiency, colour purity, reliability and cost-effective fabrication1-4. Intensive efforts have produced red-, green- and blue-emitting QD-LEDs with efficiencies of 20.5 per cent4, 21.0 per cent5 and 19.8 per cent6, respectively, but it is still desirable to improve the operating stability of the devices and to replace their toxic cadmium composition with a more environmentally benign alternative. The performance of indium phosphide (InP)-based materials and devices has remained far behind those of their Cd-containing counterparts. Here we present a synthetic method of preparing a uniform InP core and a highly symmetrical core/shell QD with a quantum yield of approximately 100 per cent. In particular, we add hydrofluoric acid to etch out the oxidative InP core surface during the growth of the initial ZnSe shell and then we enable high-temperature ZnSe growth at 340 degrees Celsius. The engineered shell thickness suppresses energy transfer and Auger recombination in order to maintain high luminescence efficiency, and the initial surface ligand is replaced with a shorter one for better charge injection. The optimized InP/ZnSe/ZnS QD-LEDs showed a theoretical maximum external quantum efficiency of 21.4 per cent, a maximum brightness of 100,000 candelas per square metre and an extremely long lifetime of a million hours at 100 candelas per square metre, representing a performance comparable to that of state-of-the-art Cd-containing QD-LEDs. These as-prepared InP-based QD-LEDs could soon be usable in commercial displays.

Highly efficient and stable InP/ZnSe/ZnS quantum dot light-emitting diodes

Colloidal quantum dot (QD) solids are emerging semiconductors that have been actively explored in fundamental studies of charge transport1 and for applications in optoelectronics2. Forming high-quality QD solids—necessary for device fabrication—requires substitution of the long organic ligands used for synthesis with short ligands that provide increased QD coupling and improved charge transport3. However, in perovskite QDs, the polar solvents used to carry out the ligand exchange decompose the highly ionic perovskites4. Here we report perovskite QD resurfacing to achieve a bipolar shell consisting of an inner anion shell, and an outer shell comprised of cations and polar solvent molecules. The outer shell is electrostatically adsorbed to the negatively charged inner shell. This approach produces strongly confined perovskite QD solids that feature improved carrier mobility (≥0.01 cm2 V−1 s−1) and reduced trap density relative to previously reported low-dimensional perovskites. Blue-emitting QD films exhibit photoluminescence quantum yields exceeding 90%. By exploiting the improved mobility, we have been able to fabricate CsPbBr3 QD-based efficient blue and green light-emitting diodes. Blue devices with reduced trap density have an external quantum efficiency of 12.3%; the green devices achieve an external quantum efficiency of 22%. A solution-based ligand-exchange strategy enables the realization of close-packed quantum dot solid films with near-unity photoluminescence quantum yield and high charge carrier mobility.

Bipolar-shell resurfacing for blue LEDs based on strongly confined perovskite quantum dots

In quantum-confined semiconductor nanostructures, electrons exhibit distinctive behavior compared with that in bulk solids. This enables the design of materials with tunable chemical, physical, electrical, and optical properties. Zero-dimensional semiconductor quantum dots (QDs) offer strong light absorption and bright narrowband emission across the visible and infrared wavelengths and have been engineered to exhibit optical gain and lasing. These properties are of interest for imaging, solar energy harvesting, displays, and communications. Here, we offer an overview of advances in the synthesis and understanding of QD nanomaterials, with a focus on colloidal QDs, and discuss their prospects in technologies such as displays and lighting, lasers, sensing, electronics, solar energy conversion, photocatalysis, and quantum information.

Semiconductor quantum dots: Technological progress and future challenges

Quantum dot light-emitting diodes are promising light sources for applications in displays. However, to date, there have been no reports of devices that simultaneously offer both high brightness and high external quantum efficiency. Here, we report red, green and blue quantum dot light-emitting diodes based on CdSe/ZnSe core/shell structures that have these attributes. We demonstrate devices with maximum external quantum efficiencies of 21.6%, 22.9% and 8.05% for red, green and blue colours with corresponding brightness of 13,300 cd m–2, 52,500 cd m–2 and 10,100 cd m–2. The devices also offer peak luminance of 356,000 cd m–2, 614,000 cd m–2 and 62,600 cd m–2, respectively. We postulate that this high performance is due to the use of Se throughout the core/shell regions and the existence of alloyed bridging layers at the core/shell interfaces. This study suggests that in the future visible quantum dot light-emitting diodes will also be suitable for lighting applications. Red, green and blue CdSe/ZnSe quantum dot light-emitting diodes combine efficient operation with high brightness.

Visible quantum dot light-emitting diodes with simultaneous high brightness and efficiency

Low-cost and efficient electrocatalysts are urgently required for the N2 reduction reaction (NRR) to produce NH3 under ambient conditions. By using first-principles calculation, we systematically i...

Computational Evaluation of Electrocatalytic NitrogenReduction on TM Single‑, Double‑, and Triple-Atom Catalysts(TM = Mn, Fe, Co, Ni) Based on Graphdiyne Monolayers

In the present work, we investigated theoretically the linear, nonlinear, and total absorption coefficients and refractive index changes associated with intersubband transitions in ZnO/ZnS core shell quantum dot (CSQD) and ZnS/ZnO inverted CSQD (ICSQD), emphasizing on the influence of the shell thickness, impurity, and dielectric environment. The effect of the polarization charges due to the possible existence of the dielectric mismatch between the system and its surrounding matrix is considered. The electronic structures are numerically calculated by employing the potential morphing method in the framework of effective mass approximation. We find that in both impurity-free CSQD and ICSQD, increasing the shell thickness red shifts significantly the threshold energy and enhances drastically the nonlinear absorption coefficients and all the refractive index changes, independently on the dielectric environments. Similar behaviour has also been observed in most of the cases studied when the impurity is displaced from the core center to the shell center. In contrast, comparing to a dielectrically homogeneous system, dispersing the systems into a matrix with a lower dielectric constant blue shifts all the peak positions of the absorption coefficients and refractive index changes. However, the corresponding magnitudes (in absolute value) are substantially reduced. Finally, we find that the nonlinear properties are more sensitive to the external perturbations, while at a weak radiation intensity, the variation of the total quantities is generally dominated by that of the corresponding linear terms.

Linear and nonlinear optical properties of ZnO/ZnS and ZnS/ZnO core shell quantum dots: Effects of shell thickness, impurity, and dielectric environment

Zaiping Zeng

Papers

Visible quantum dot light-emitting diodes with simultaneous high brightness and efficiency

Computational Evaluation of Electrocatalytic NitrogenReduction on TM Single‑, Double‑, and Triple-Atom Catalysts(TM = Mn, Fe, Co, Ni) Based on Graphdiyne Monolayers

Linear and nonlinear optical properties of ZnO/ZnS and ZnS/ZnO core shell quantum dots: Effects of shell thickness, impurity, and dielectric environment

High-Efficiency Green InP Quantum Dot-Based Electroluminescent Device Comprising Thick-Shell Quantum Dots

Theoretical screening of the transition metal heteronuclear dimer anchored graphdiyne for electrocatalytic nitrogen reduction