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At least 91 records · Page 5

Excited-State Charge Distribution of a Donor–π–Acceptor Zn Porphyrin Probed by N K-Edge Transient Absorption Spectroscopy

Zinc porphyrin solar cell dyes with donor-π–acceptor architectures combine light absorber (π), electron-donor, and electron-acceptor moieties inside a single molecule with atomic precision. The donor-π–acceptor design promotes the separation of charge carriers following optical excitation. Here, we probe the excited-state electronic structure within such molecules by combining time-resolved X-ray absorption spectroscopy at the N K-edge with first-principles time-dependent density functional theory (TD-DFT) calculations. Furthermore, customized Zn porphyrins with strong-donor triphenylamine groups or weak-donor tri-tert-butylbenzene groups were synthesized. Energetically well-separated N K-edge absorption features simultaneously probe the excited-state electronic structure from the perspectives of the macrocycle and triphenylamine N atoms. New absorption transitions between the macrocycle N atoms and the excited-state HOMO vacancy are observed, and the triphenylamine associated absorption feature blue-shifts, consistent with partial oxidation of the donor groups in the excited state.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Modeling electric charge distribution on insulator under electron bombardment: Case of rectangular surface implantation

Despite progress in the study of dielectric properties and the formation of secondary electrons images and especially in the understanding of their mirror curve shape, since the first models for mirror equation were developed, an exact quantitative prediction of the mirror curve for most materials has remained an unsolved problem. In this paper, recent development in the characterization of charge trapping ability of insulators using the scanning electron microscope mirror method (SEMMM) is reviewed. All this work has resulted in unprecedented insights into the early stage of dielectric study and it is also relevant for a deeper understanding of this anomalous effect (mirror effect) as well as for discussion of the factors affecting it. So the dependency of elliptic mirror and the anisotropic effect in the trapping phenomena of charge is highlighted.

36 MATERIALS SCIENCE↗

Mapping hidden space-charge distributions across crystalline metal oxide/group IV semiconductor interfaces

The electronic structures of semiconducting heterojunctions are critically dependent on composition including the presence and concentrations of dopants, both intended and unintended. Dopant profiles in the interfacial region can have major effects on band energies which in turn drive transport properties. Here, in this study, we use core-level photoelectron line shapes excited with hard x rays to extract information about electric fields resulting from internal charge transfer in epitaxial La 0.03 Sr 0.97 Zr x Ti 1–x O 3 /Ge(001) (0.1≤x≤0.7) heterostructures. Experiments were carried out for heterojunctions involving both n- and p-type Ge substrates. These heterojunctions were not amenable to electronic characterization of all regions by transport measurements because the doped substrates act as electrical shunts, precluding probing the more resistive films and masking interface conductivity. However, the core-level line shapes were found to be a rich source of information on built-in potentials that exist throughout the heterostructure, and yielded valuable insight into the impact of band bending on band alignment at the buried interfaces. The electronic effects expected for Ge with uniform n- and p-type doping are eclipsed by those of unintended oxygen dopants in the Ge near the interface. This study illustrates the power of hard x-ray photoemission spectroscopy and related modeling to determine electronic structure in material systems for which insight from traditional transport measurements is limited.

36 MATERIALS SCIENCE↗

Charge distribution in lightning flashes

Four VHF receivers about 10 km apart were used to detect three-dimensional lightning VHF sources during active thunderstorms. A computer implemented algorithm was used to determine the difference in the time of arrival (DTOA) between the VHF pulses. The three-dimensional source locations determined from the DTOA were correlated with ground electric field measurements (0.1 Hz to 1.5 MHz). Four cloud to ground (CG) and three intracloud (IC) flashes, selected randomly, were studied. A point charge model was used to determine the charge being removed during the different phases of CG and IC flashes. It was determined that return strokes lowered between 24.1 and 3.6 coulombs of negative charge to ground from heights between 10.5 and 5.8 km above MSL. The interstroke process after the first return stroke in a CG flash lowered between 3.4 and 0.9 coulombs of negative charge between the heights of 14.2 (near the cloud tops) to heights of 5.8 km (near the beginning of the leader-return stroke process).

Rustan, P. L.↗

Stable dielectric charge distributions from field enhancement of secondary mission

The emission of secondary electrons from dielectrics subject to numerous effects of electric field which are experimentally difficult to control is discussed. Measurements are reported using pulse techniques such that local fields do not build to significant levels, but measurements with fields present are also of interest. A specific series of measurements under controlled conditions are described and their implications in terms of fields, magnitude and angle, near the dielectric surface were examined. The measurements were made for a charged fluorinated-ethylene-propylene surface near a grounded aluminum half-round resting on the surface. The geometry produced a stable surface-charge gradient being controlled by a strongly enhanced secondary emission for which a model is constructed. Observations of surface flashovers under various conditions confirm the predictions of some scaling exercises.

Robinson, J. W.↗

Mars Dust: Characterization of Particle Size and Electrostatic Charge Distributions

Some of the latest pictures of Mars surface sent by NASA s Spirit rover in early January, 2004, show very cohesive, mud-like dust layers. Significant amounts of dust clouds are present in the atmosphere of Mars. NASA spacecraft missions to Mars confirmed hypotheses from telescopic work that changes observed in the planet s surface markings are caused by wind-driven redistribution of dust. In these dust storms, particles with a wide range of diameters (< 1 m to 50 m) are a serious problem to solar cells, spacecraft, and spacesuits. Dust storms may cover the entire planet for an extended period of time. It is highly probable that the particles are charged electrostatically by triboelectrification and by UV irradiation.

Mazumder, M. K.↗

Mars Dust: Characterization of Particle Size and Electrostatic Charge Distribution

Some of the latest pictures of Mars surface sent by NASA's Spirit rover in early January, 2004, show very cohesive, "mud-like" dust layers. Significant amounts of dust clouds are present in the atmosphere of Mars [1-4]. NASA spacecraft missions to Mars confirmed hypotheses from telescopic work that changes observed in the planet's surface markings are caused by wind-driven redistribution of dust. In these dust storms, particles with a wide range of diameters (less than 1 micrometer to 50 micrometers) are a serious problem to solar cells, spacecraft, and spacesuits. Dust storms may cover the entire planet for an extended period of time [5]. It is highly probable that the particles are charged electrostatically by triboelectrification and by UV irradiation.

Mazumder, M. K.↗

Excited state charge distribution and bond expansion of ferrous complexes observed with femtosecond valence-to-core x-ray emission spectroscopy

Valence-to-core x-ray emission spectroscopy (VtC XES) combines the sample flexibility and element specificity of hard x-rays with the chemical environment sensitivity of valence spectroscopy. Here, we extend this technique to study geometric and electronic structural changes induced by photoexcitation in the femtosecond time domain via laser-pump, x-ray probe experiments using an x-ray free electron laser. The results of time-resolved VtC XES on a series of ferrous complexes [Fe(CN) 2n (2, 2'-bipyridine) 3-n ] -2n+2 , n = 1, 2, 3, are presented. Comparisons of spectra obtained from ground state density functional theory calculations reveal signatures of excited state bond length and oxidation state changes. An oxidation state change associated with a metal-to-ligand charge transfer state with a lifetime of less than 100 fs is observed, as well as bond length changes associated with metal-centered excited states with lifetimes of 13 ps and 250 ps.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Erratum to: Measurements of higher-order cumulants of multiplicity and net-electric charge distributions in inelastic proton-proton interactions by NA61/SHINE

This Erratum replaces, due to a discovery of coding mistakes, the following quantities: κ 3 /κ 1 of the h + − h − distribution presented in Fig. 6 and Table 6, κ 4 listed in Table 4, and $\hat{C}$ 4 presented in Fig. 7 and Table 5. All mentioned figures and tables were updated.

High-Energy Particle Collision Data Analysis↗

Polarization-dependent infrared reflectivity study of Sr 2.5 Ca 11.5 Cu 24 O 41 under pressure: Charge dynamics, charge distribution, and anisotropy

We present a polarization-dependent infrared reflectivity study of the spin-ladder compound Sr₂̣₅Ca₁₁̣₅Cu₂₄O₄₁ under pressure. The optical response is strongly anisotropic, with the highest reflectivity along the ladders/chains ( E ∥c) revealing a metallic character. For the polarization direction perpendicular to the ladder plane, an insulating behavior is observed. With increasing pressure the optical conductivity for E ∥c shows a strong increase, which is most pronounced below 2000cm⁻¹. According to the spectral weight analysis of the E ∥c optical conductivity the hole concentration in the ladders increases with increasing pressure and tends to saturate at high pressure. At ~7.5 GPa the number of holes per Cu atom in the ladders has increased by Δδ=0.09(±0.01), and the Cu valence in the ladders has reached the value +2.33. Thus, the optical data suggest that Sr₂̣₅Ca₁₁̣₅Cu₂₄O₄₁ remains electronically highly anisotropic up to high pressure, also at low temperatures.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗