Covalent modification of a glassy carbon surface by 4-aminobenzoic acid and its application in fabrication of a polyoxometalates-consisting monolayer and multilayer films

4-Aminobenzoic acid (4-ABA) was covalently grafted on a glassy carbon electrode (GCE) by amine cation radical formation in the electrooxidation process of the amino-containing compound. X-ray photoelectron spectroscopy measurement proves the presence of 4-carboxylphenylamine monolayer on the GCE. The redox responses of various electroactive probes were investigated on the 4-ABA-modified GCE. Electron transfer to Fe(CN)(6)(3-) in solutions of various pHs was studied by both cyclic voltammetry and electrochemical impedance analysis on the modified electrode. Changes in the solution pH value result in the variation of the terminal group charge state, based on which surface pK(a) values are estimated. The 4-ABA-modified GCE was used as a suitable charged substrate to fabricate polyoxometalates-consisting (POM-consisting) monolayer and multilayer films through layer-by-layer assembly based on electrostatic attraction. Cyclic voltammetry shows the uniform growth of these three-dimensional multilayer films. Taking K10H3[Pr-(SiMo7W4O39)(2)]. H2O (abbreviated as Pr(SiMo7W4)(2)), for example, the preparation and electrochemical behavior of its monolayer and multilayer film had been investigated in detail. This modification strategy is proven to be a general one suitable for anchoring many kinds of POMs on the 4-ABA-modified GCE.

Gas-phase ion - Molecule reactions of neutral C-60 with the plasmas of alkyl methyl ethers and primary alcohols

The gas-phase ion-molecule reactions of C-60 with the methoxymethyl ion [CH3O=CH2](+) and the 1-hydroxyethyl ion [CH3CH=OH](+) generated under the self-chemical-ionization (self-CI) conditions of alkyl methyl ethers and primary alcohols were studied in the ion source of a mass spectrometer. The adduct ions [C60C2H5O](+) and protonated molecules [C60H](+) were observed as the major products of C-60 with the plasma of alkyl methyl ethers. On the contrary, the reactions of C-60 With the plasmas of primary alcohols produced few corresponding adduct ions. The AM1 semiempirical molecular orbital calculations were carried out on 14 possible structures. The calculated results showed that the most stable structure among the possible isomers of [C60C2H5O](+) is the [3+2] cycloadduct. According to experimental and theoretical results, the pathway for the formation of the adduct was presented.

Synthesis, extraction and electronic structure of Ce@C-2n

In view of the growing interest in endohedral lanthanide fullerenes, Ce, as a typical +4 oxidation state lanthanide element, has been systematically studied. The synthesis, extraction and electronic structure of Ce@C-2n are investigated. Soot containing Ce@C-2n was synthesized in high yield by carbonizing CeO2-containing graphite rods and are back-burning the CeC2-enriched cathode deposit in a DC are plasma apparatus. Ce@C-2n, dominated by Ce@C-82, can be efficiently extracted from the insoluble part of the soot after toluene Soxhlet extraction by pyridine at high temperature and high pressure in a closed vessel. About 60% Ce@C-2n (2n = 82,80,78,76) and 35% Ce@C-82 can be enriched in the pyridine extract. This fact is identified by desorption electron impact mass spectrometry (DEI MS). The electronic structure of Ce@C-2n is analyzed by using X-ray photoemission spectroscopy (XPS) of pyridine-free film. It is suggested that the encapsulated Ce atom is in a charge state close to +3 and was effectively protected from reaction with water and oxygen by the enclosing fullerene cage. Unlike theoretical expectation, the electronic state of Ce@C-82 is formally described as Ce+3@C-82(3-). (C) 1997 Elsevier Science Ltd.

Reduced dynamics with renormalization in solid-state charge qubit measurement

Quantum measurement will inevitably cause backaction on the measured system, resulting in the well-known dephasing and relaxation. In this paper, in the context of solid-state qubit measurement by a mesoscopic detector, we show that an alternative backaction known as renormalization is important under some circumstances. This effect is largely overlooked in the theory of quantum measurement.

Continuous weak measurement and feedback control of a solid-state charge qubit: A physical unravelling of non-Lindblad master equation

Conventional quantum trajectory theory developed in quantum optics is largely based on the physical unravelling of a Lindblad-type master equation, which constitutes the theoretical basis of continuous quantum measurement and feedback control. In this work, in the context of continuous quantum measurement and feedback control of a solid-state charge qubit, we present a physical unravelling scheme of a non-Lindblad-type master equation. Self-consistency and numerical efficiency are well demonstrated. In particular, the control effect is manifested in the detector noise spectrum, and the effect of measurement voltage is discussed.

Quantum coherence control of solid-state charge qubit by means of a suboptimal feedback algorithm

The quantum coherence control of a solid-state charge qubit is studied by using a suboptimal continuous feedback algorithm within the Bayesian feedback scheme. For the coherent Rabi oscillation, the present algorithm suggests a simple bang-bang control protocol, in which the control parameter is modulated between two values. For the coherence protection of the idle state, the present approach is applicable to arbitrary states, including those lying on the equator of the Bloch sphere which are out of control in the previous Markovian feedback scheme.

Enhancement of three-photon absorption cross-sections in a novel class of symmetrical charge transfer fluorene-based molecules

The three-photon absorption effect (3PA) of two novel symmetrical charge transfer fluorene-based molecules (abbreviated as BASF and BMOSF) has been determined by using a Q-switched Nd:YAG laser pumped with 38 ps pulses at 1064 nm in DMF. The measured 3PA cross-sections are 84 x 10(-78) and 114 x 10(-78) cm(6) s(2), respectively. The geometries and electronic excitations of these two molecules are systematically studied by PM3 and ZINDO/S methods. The relationships between 3PA cross-sections and intramolecular charge transfer are discussed micromechanically. The experimental and theoretical results have shown that the larger intramolecular charge transfer, which was characterized by the charge density difference between the ground state (SO) and the first excited state (S-I), the greater enhancement of the 3PA cross-sections. (c) 2005 Elsevier B.V. All rights reserved.

Theoretical investigation on the one- and two-photon absorption properties for a series of symmetrical charge transfer fluorene-phenylene and fluorene-thiophene derivatives

One- and two-photon absorption properties of a series of fluorene derivatives with symmetrical charge transfer D-IT-D and A-IT-A structural motifs have been theoretically investigated with ZINDO/S method. The optimized structures and the characterization of frontier molecular orbitals were obtained by using AMI calculations. Two-photon absorption properties of molecules have been studied using three-state model. The calculation results have shown that fluorene-thiophene derivatives exhibit larger two-photon absorption cross-section as compared with other studied molecules. To illustrate the results, the crucial effects of thiophene ring on fluorenethiophene derivatives and the net charge changes on the pi-conjugated bridges are analyzed theoretically. (c) 2006 Elsevier B.V. All rights reserved.

Mechanical and chemical bonding properties of ground state BeH2

The crystal structure, mechanical properties and electronic structure of ground state BeH2 are calculated employing the first-principles methods based on the density functional theory. Our calculated structural parameters at equilibrium volume are well consistent with experimental results. Elastic constants, which well obey the mechanical stability criteria, are firstly theoretically acquired. The bulk modulus B, Shear modulus G, Young's modulus E, and Poisson's ratio upsilon are deduced from the elastic constants. The bonding nature in BeH2 is fully interpreted by combining characteristics in band structure, density of states, and charge distribution. The ionicity in the Be-H bond is mainly featured by charge transfer from Be 2s to H 1s atomic orbitals while its covalency is dominated by the hybridization of H 1s and Be 2p states. The Bader analysis of BeH2 and MgH2 are performed to describe the ionic/covalent character quantitatively and we find that about 1.61 (1.6) electrons transfer from each Be (Mg) atom to H atoms.

Theoretical analysis and experimental study of the space-charge-screening effect in uni-traveling-carrier photodiode

A new optimized structure of an UTC (uni-traveling-carrier) photodiode is developed and epitaxied by metal-organic chemical vapor deposition. We fabricated a UTC photodiode of 30 mu m in diameter. Theoretical simulation based on drift-diffusion model was used to analyze the space-charge-screening effect in UTC photodiode primarily in two aspects: the carrier concentrations and the space electric field. The simulation results were generally in agreement with the experimental data.

Space-charge-limited currents in GaN Schottky diodes

Unusual dark current voltage (I-V) characteristics were observed in GaN Schottky diodes. I-V characteristics of the GaN Schottky diodes were measured down to the magnitude of 10(-14) A. Although these Schottky diodes were clearly rectifying, their I-V characteristics were non-ideal which can be judged from the non-linearity in the semi-logarithmic plots. Careful analysis of the forward bias I-V characteristics on log-log scale indicates space-charge-limited current (SCLC) conduction dominates the current transport in these GaN Schottky diodes. The concentration of the deep trapping centers was estimated to be higher than 10(15) cm(-3). In the deep level transient spectra (DLTS) measurements for the GaN Schottky diodes, deep defect levels around 0.20 eV below the bottom of the conduction band were identified, which may act as the trapping centers. The concentration of the deep centers obtained from the DLTS data is about 5 x 10(15) cm(-3). SCLC measurements may be used to probe the properties of deep levels in wide bandgap GaN-AlGaN compound semiconductors, as is the case with insulators in the presence of trapping centers. (c) 2005 Elsevier Ltd. All rights reserved.

Simulation research of nonlinear behavior induced by the charge-carrier effect in resonant-cavity-enhanced photodetectors

In this paper, we have calculated and discussed in detail the nonlinear effect induced by three carrier effects: free-carrier absorption, bandgap filling, and bandgap shrinkage. The central wavelength of response of resonant-cavity-enhanced (RCE) photodetectors shifts according to the change of the refractive index, and the response of a given optical wavelength simultaneously changes.With an increasing As composition of ln(1-x)Ga(x)As(y)P(1-y) and the spacer thickness, the nonlinear effect increases, but the -1-dB input saturation optical power and the -1-dB saturation photocurrent decrease. Bistable-state operation occurs when the input optical power is in the proper bistable region.

Mode softening in charge-density excitations of a two-dimensional electron gas driven by Rashba spin-orbit interaction

The electron density response of a uniform two-dimensional (2D) electron gas is investigated in the presence of a perpendicular magnetic field and Rashba spin-orbit interaction (SOI). It is found that, within the Hartree-Fock approximation, a charge density excitation mode below the cyclotron resonance frequency shows a mode softening behavior, when the spin-orbit coupling strength falls into a certain interval. This mode softening indicates that the ground state of an interacting uniform 2D electron gas may be driven by the Rashba SOI to undergo a phase transition to a nonuniform charge density wave state.

Quantum measurement of single electron state by a quantum point contact

Closely related to the quantum information processing in solid states, we study the quantum measurement of single electron state by a mesoscopic charge-sensitive detector, namely the quantum point contact (QPC). We find that the conventional Lindblad-type master equation is not appropriate for describing the underlying measurement dynamics. The treatment developed in this work properly accounts for the energy-exchange between the detector and the measured system, and its role on the detailed-balance relation. A valid description for the QPC measurement dynamics is provided which may have impact on the study of quantum measurement and quantum feedback control in solid states.

A Fast-Locking Phase-Locked Loop Using a Seven-State Phase Frequency Detector

A seven-state phase frequency detector (S.S PFD) is proposed for fast-locking charge pump based phase-locked loops (CPPLLs) in this paper. The locking time of the PLL can be significantly reduced by using the seven-state PFD to inject more current into the loop filter. In this stage, the bandwidth of the PLL is increased or decreased to track the phase difference of the reference signal and the feedback signal. The proposed architecture is realized in a standard 0.35 mu m 2P4M CMOS process with a 3.3V supply voltage. The locking time of the proposed PLL is 1.102 mu s compared with the 2.347 mu s of the PLL based on continuous-time PFD and the 3.298 mu s of the PLL based on the pass-transistor tri-state PFD. There are 53.05% and 66.59% reductions of the locking time. The simulation results and the comparison with other PLLs demonstrate that the proposed seven-state PFD is effective to reduce locking time.