Injection, Transport, Absorption and Phosphorescence Properties of a Series of Blue-Emitting Ir(III) Emitters in OLEDs: a DFT and Time-Dependent DFT Study

Quantum-chemistry methods were explored to investigate the electronic structures, injection and transport properties, absorption and phosphorescence mechanism of a series of blue-emitting Ir(III) complexes {[(F-2-ppy)(2)Ir(pta -X/pyN4)], where F-2-ppy = (2,4-difluoro)phenylpyridine; pta = pyridine-1,2,4-triazole; X = phenyl(1); p-tolyl (2); 2,6-difluororophenyl (3); -CF3 (4), and pyN4 = pyridine-1,2,4-tetrazolate (5)}, which are used as emitters in organic light-emitting diodes (OLEDs). The mobility of hole and electron were studied computationally based on the Marcus theory. Calculations of Ionization potentials (IPs) and electron affinities (EAs) were used to evaluate the injection abilities of holes and electrons into these complexes.

Different electronic structures and spectroscopic properties of cationic [M(ppy)2(N--N)]+ (M = Rh, Ir; N--N = Hcmbpy, H2dcbpy), a DFT study.

We report a comparative quantum-chemical study of the electronic structures and optical properties of a series of cationic complexes [M(ppy)(2)(N--N)](+) (N--N = Hcmbpy = 4-carboxy-4'-methylbpy, M = Rh (Rh1), Ir(Ir2); N--N = H(2)dcbpy = 4,4'-dicarboxy-bpy, M = Rh (Rh3) and Ir (Ir4)). The theoretical calculation reveals that the increased number of -COOH groups on the bpy ligand can decrease the energy levels of LUMO more than HOMO and narrow down the HOMO-LUMO energy gaps, which results in the red-shifted of the lowest-lying absorption and phosphorescent spectra. The lowest-lying singlet absorptions were categorized as d(M,M = Rh or Ir) + pi(ppy) -->pi*(bpy) with MLCT and LLCT characters.

Pressure Effects on the Structural, Electronic, and Optical Properties of Si-n@SWCNTs

Well-ordered single, double/four parallel, three/four-strands helical chains, and five-strand helical chain with a single atom chain at the center of Si nanowires (NWs) inside single-walled carbon nanotubes (Si-n@SWCNTs) are obtained by means of molecular dynamics. On the basis of these optimized structures, the structural evolution of Si-n@SWCNTs subjected to axial stress at low temperature is also investigated. Interestingly, the double parallel chains depart at the center and transform into two perpendicular parts, the helical shell transformed into chain, and the strand number of Si NWs increases during the stress load. Through analyzis of pair correlation function (PCF), the density of states (DOS), and the z-axis polarized absorption spectra of Si-n@SWCNTs, we find that the behavior of Si-n@SWCNTs under stress strongly depends on SWCNTs' symmetry, diameter, as well as the shape of Nws, which provide valuable information for potential application in high pressure cases such as seabed cable.

Electronic structures and chemical bonding in transition metal monosilicides MSi (M=3d, 4d, 5d elements)

Bond distances, vibrational frequencies, electron affinities, ionization potentials, dissociation energies, and dipole moments of the title molecules in neutral, positively, and negatively charged ions were studied using the density functional method. Ground state was assigned for each species. The bonding patterns were analyzed and compared with both the available data and across the series. It was found that besides an ionic component, covalent bonds are formed between the metal s, d orbitals and the silicon 3p orbital. The covalent character increases from ScSi (YSi) to NiSi (PdSi) for 3d (4d) metal monosilicides, then decreases. For 5d metal monosilicides, the covalent character increases from LaSi to OsSi, then decreases. For the dissociation of cations, the dissociation channel depends on the magnitude of the ionization potential between metal and silicon. If the ionization potential of the metal is smaller than that of silicon, channel MSi+-> M++Si is favored. Otherwise, MSi+-> M+Si+ will be favored. A similar behavior was observed for anions, in which the dissociation channel depends on the magnitude of electron affinity.

Substitution effect of nitrogen atoms with carbon atoms in porphyrin on the electronic structure and excited states properties

Density functional theory (DFT) electronic structure calculations were carried out to predict the structures and the absorption and emission spectra for porphyrin and a series of carbaporphyrins-carbaporphyrin, adj-dicarbaporphyrin, opp-dicarbaporphyrin, tricarbaporphyrin and tetracarbaporphyrin. The ground- and excited-state geometries were optimized at the B3LYP/6-31g(d) and CIS/6-31g(d) level, respectively. The optimized ground-state geometry and absorption spectra of porphyrin, calculated by DFT and time-dependent DFT (TDDFT), are comparable with the available experimental values. Based on the optimized excited-state geometries obtained by CIS/6-31g(d) method, the emission properties are calculated using TDDFT method at the B3LYP/6-31g(d) level. The effects of the substitution of nitrogen atoms with carbon atoms at the center positions of porphyrin are discussed. The results indicate that the two-pyrrole nitrogens are important to the chemical and physical properties for porphyrin.

Partition Energy Absorption of Axially Crushed Aluminum Foam-Filled Hat Sections

The "interaction effect" between aluminum foam and metal column that takes place when foam-filled hat sections (top-hats and double-hats) are axially crushed was investigated in this paper. Based on experimental examination, numerical simulation and analytical models, a systemic approach was developed to partition the energy absorption quantitatively into the foam filler component and the hat section component, and the relative contribution of each component to the overall interaction effect was therefore evaluated. Careful observation of the collapse profile found that the crushed foam filler could be further divided into two main energy-dissipation regions: densified region and extremely densified region. The volume reduction and volumetric strain of each region were empirically estimated. An analytical model pertinent to the collapse profile was thereafter proposed to find the more precise relationship between the volume reduction and volumetric strain of the foam filler. Combined the superfolding element model for hat sections with the current model according to the coupled method, each component energy absorption was subsequently derived, and the influence of some controlling factors was discussed. According to the finite element analysis and the theoretical modeling, when filled with foam, energy absorption was found to be increased both in the hat section and the foam filler, whereas the latter contributes predominantly to the interaction effect. The formation of the extremely densified region in the foam filler accounts for this effect.

Theermal Stress and Fracture in Transparent Optical Materials due to Laser Energy-Absorption by a Defect

利用热弹性理论分析了在光学材料中由于缺陷吸收激光能量引起的温度和热应力分布,并且针对一个简单的裂纹模型分析了热应力产生的应力强度因子,给出了一些主要参数对于应力强度因子的影响的规律。

Numerical Partition of Energy Absorption of Foam-filled Top-Hat and Double-Hat Sections

The interaction effect, i.e., the contribution of each component to the total energy absorption of an axially crushed foam-filled hat section was investigated quantitatively via numerical simulation. The FE results were first verified by experimental work of aluminum foam-filled top-hat and double-hat sections, then the contribution of foam-fillers and that of hat sections to the overall energy absorption were quantitatively obtained, respectively. When foam-filled, increase in energy absorption was found both in hat section component and foam-filler component, whereas the latter contributes predominantly to the interaction effect.

A Wide Band Strong Acoustic Absorption in a Locally Network Anechoic Coating

Composite materials with interpenetrating network structures usually exhibit unexpected merit due to the cooperative interaction. Locally resonant phononic crystals (LRPC) exhibit excellent sound attenuation performance based on a periodical arrangement of sound wave scatters. Inspired by the interpenetrating network structure and the LRPC concept, we develop a locally network anechoic coating (LNAC) that can achieve a wide band of underwater strong acoustic absorption. The experimental results show that the LNAC possesses an excellent underwater acoustic absorbing capacity in a wide frequency range. Moreover, in order to investigate the impact of the interpenetrating network structure, we fabricate a faultage structure sample and the network is disconnected by hard polyurethane (PU). The experimental comparison between the LNAC and the faultage structure sample shows that the interpenetrating network structure of the LNAC plays an important role in achieving a wide band strong acoustic absorption.

Effects of spontaneously induced coherence on absorption of a ladder-type atom

This paper investigates the effects of spontaneously induced coherence on absorption properties in a nearly equispaced three-level ladder-type system driven by two coherent fields. It find that the absorption properties of this system with the probe field applied on the lower transition can be significantly modified if this coherence is optimized. In the case of small spontaneous decay rate in the upper excited state, it finds that such coherence does not destroy the electromagnetically induced transparency (EIT). Nevertheless, the absorption peak on both sides of zero detuning and the linewidth of absorption line become larger and narrower than those in the case corresponding to the effects of spontaneously induced coherence; while in the case of large decay rate, it finds that, instead of EIT with low resonant absorption, a sharp absorption peak at resonance appears. That is, electromagnetically induced absorption in the nearly equispaced ladder-type system can occur due to such coherent effects.

Electronic entanglement purification scheme enhanced by charge detections

We present an entanglement purification scheme for the mixed entangled states of electrons with the aid of charge detections. Our scheme adopts the electronic polarizing beam splitters rather than the controlled-NOT (CNOT) operations, but the total successful probability of our scheme can reach the quantity as large as that of the the CNOT-operation-based protocol and twice as large as that of linear-optics-based protocol for the purification of photonic entangled states. Thus our scheme can achieve a high successful prabability without the usage of CNOT operations.

Polaronic correction to the first excited electronic energy level in an anisotropic semiconductor quantum dot

Within the framework of second-order Rayleigh-Schrodinger perturbation theory, the polaronic correction to the first excited state energy of an electron in an quantum dot with anisotropic parabolic confinements is presented. Compared with isotropic confinements, anisotropic confinements will make the degeneracy of the excited states to be totally or partly lifted. On the basis of a three-dimensional Frohlich's Hamiltonian with anisotropic confinements, the first excited state properties in two-dimensional quantum dots as well as quantum wells and wires can also be easily obtained by taking special limits. Calculations show that the first excited polaronic effect can be considerable in small quantum dots.

Ultrafast electronic excitation in CaF2 crystals

A new pump and probe experimental system was developed, the pump pulse duration of which is stretched and is much longer than that of the probe pulse. Using this system, time-resolved electronic excitation processes and damage mechanisms in CaF2 crystals were studied. The measured reflectivity of the probe pulse begins to increase at the peak of the pump pulse and increases rapidly in the latter half of the pump pulse, when the pump pulse duration is stretched to 580fs. Our experimental results indicate that both multiphoton ionization and impact ionization play important roles in the generation of conduction band electrons, at least they do so when the pump pulse durations are equal to or longer than 580fs.

Phase-dependent properties for absorption and dispersion in a closed equispaced three-level ladder system

It is shown that in a closed equispaced three-level ladder system, by controlling the relative phase of two applied coherent fields, the conversion from absorption with inversion to lasing without inversion (LWI) can be realized; a large index of the refraction with zero absorption can be gotten; considerable increasing of the spectrum region and value of the LWI gain can be achieved. Our study also reveals that the incoherent pumping will produce a remarkable effect oil the phase-dependent properties of the system. Modifying value of the incoherent pumping can change the property of the system from absorption to amplification and enhance significantly LWI gain. If the incoherent pumping is absent, we cannot get any gain for any value of the relative phase. (c) 2007 Elsevier GmbH. All rights reserved.

Simultaneous three-photon absorption induced ultraviolet upconversion in Pr3+:Y2SiO5 crystal by femtosecond laser irradiation

Near-infrared to ultraviolet upconversion luminescence was observed in the Pr3+ :Y2SiO5 crystal with 120 fs, 800 mn infrared laser irradiation. The observed emissions at around 270 nm and 305 nm could be assigned to 5d -> 4f transitions of Pr3+ ions. The relationship between the upconversion luminescence intensity and the pump power of the femtosecond laser reveals that the UV emission belongs to simultaneous three-photon absorption induced upconversion luminescence. (c) 2007 Elsevier B.V. All rights reserved.