Dynamics of quantum dissipation systems interacting with fermion and boson grand canonical bath ensembles: Hierarchical equations of motion approach

A hierarchical equations of motion formalism for a quantum dissipation system in a grand canonical bath ensemble surrounding is constructed on the basis of the calculus-on-path-integral algorithm, together with the parametrization of arbitrary non-Markovian bath that satisfies fluctuation-dissipation theorem. The influence functionals for both the fermion or boson bath interaction are found to be of the same path integral expression as the canonical bath, assuming they all satisfy the Gaussian statistics. However, the equation of motion formalism is different due to the fluctuation-dissipation theories that are distinct and used explicitly. The implications of the present work to quantum transport through molecular wires and electron transfer in complex molecular systems are discussed. (c) 2007 American Institute of Physics.

Strain-Compensated InGaAs/InAlAs Quantum Cascade Detector of 4.5 mu m Operating at Room Temperature

We present a strain-compensated InP-based InGaAs/InAlAs photovoltaic quantum cascade detector grown by solid source molecular beam epitaxy. The detector is based on a vertical intersubband transition and electron transfer on a cascade of quantum levels which is designed to provide longitudinal optical phonon extraction stairs. By careful structure design and growth, the whole epilayer has a residual strain toward InP substrate of only -2.8 x 10(-4). A clear narrow band detection spectrum centered at 4.5 mu m has been observed above room temperature for a device with 200 x 200 mu m(2) square mesa.

Numerical simulation of quantum directional couplers

A numerical analysis of a quantum directional coupler based on Pi-shaped electron waveguides is presented with use of the scattering-matrix method. After the optimization of the device parameters, uniform output for the two output ports and high directivity are obtained within a wide range of the electron momenta. The electron transfer in the device is found more efficient than that in the previously proposed structures. The study of the shape-dependence of transmission for the device shows that the device structure with smooth boundaries exhibits a much better performance.

New observation on the formation of PbS clusters in zeolite-Y

PbS clusters in zeolite-Y have been prepared with the reaction of Pb2+-ion-exchanged zeolite-Y with Na2S in solution at room temperature. Their absorption spectra show dramatic blue shifts from that of the bulk PbS. Obvious change of both the absorption edges and peak positions upon PbS concentrations have been observed. These phenomena provide evidences that PbS clusters have been formed within the zeolite. The absorption spectra show featureless structure and have no tails near the absorption edges. As the PbS loading density becomes higher, the absorption bands become stronger and sharpen. Order PbS clusters lattice with high quality might be formed in the supercages of zeolite-Y. (C) 1996 American Institute of Physics.

Slow isocharged sequence ions with helium collisions: Projectile core dependence

The collisions of the isocharged sequence ions of q=6 (C6+, N6+, O6+, F6+, Ne6+, Ar6+, and Ca6+), q=7 (F7+, Ne7+, S7+, Ar7+, and Ca7+), q=8 (F8+, Ne8+, Ar8+, and Ca8+), q=9 (F9+, Ne9+, Si9+, S9+, Ar9+, and Ca9+) and q=11 (Si11+, Ar11+, and Ca11+) with helium at the same velocities were investigated. The cross-section ratios of the double-electron transfer (DET) to the single-electron capture (SEC) sigma(DET)/sigma(SEC) and the true double-electron capture (TDC) to the double-electron transfer sigma(TDC)/sigma(DET) were measured. It shows that for different ions in an isocharged sequence, the experimental cross-section ratio sigma(DET)/sigma(SEC) varies by a factor of 3. The results confirm that the projectile core is another dominant factor besides the charge state and the collision velocity in slow (0.35-0.49v(0); v(0) denotes the Bohr velocity) highly charged ions (HCIs) with helium collisions. The experimental cross-section ratio sigma(DET)/sigma(SEC) is compared with the extended classical over-barrier model (ECBM) [A. Barany , Nucl. Instrum. Methods Phys. Res. B 9, 397 (1985)], the molecular Coulombic barrier model (MCBM) [A. Niehaus, J. Phys. B 19, 2925 (1986)], and the semiempirical scaling laws (SSL) [N. Selberg , Phys. Rev. A 54, 4127 (1996)]. It also shows that the projectile core properties affect the initial capture probabilities as well as the subsequent relaxation of the projectiles. The experimental cross-section ratio sigma(TDC)/sigma(DET) for those lower isocharged sequences is dramatically affected by the projectile core structure, while for those sufficiently highly isocharged sequences, the autoionization always dominates, hence the cross-section ratio sigma(TDC)/sigma(DET) is always small.

多电荷态硫离子与氦原子和氢分子碰撞中的多电子转移过程研究

本工作采用反冲离子飞行时间技术和散射离子位置灵敏探测技术，实验研究了Sq+离子与He、H2碰撞中的多电子转移过程和分子离子的碎裂现象。研究了转移电离截面与单电子俘获截面比值和入射离子损失一个电子和两个电子的情况下，靶原子双重电离与单重电离的截面比值随入射离子能量和入射离子电荷态的变化规律，并对不同的碰撞体系的结果进行了比较。研究发现：在本工作研究的入射离子能区，对于HZ分子靶，双电子俘获自电离反应道：S2+H2→S(q-l)+2H++e-。是转移电离过程的主要贡献，而直接转移电离的贡献可以忽略；随着入射离子电荷态的增加，双电子俘获自电离的贡献增加，直接转移电离的贡献逐渐减小，但双电子俘获自电离的贡献的增加比理论预言的要慢。建立了蒙特卡罗程序模拟离子与分子碰撞中产生的具有不同的初始动能的离子碎片的飞行时间谱，深入分析和研究了Sq＋与H2分子碰撞中产生的H2+的解离过程和库仑爆炸过程，以及H＋碎片的能量分布。模拟结果与实验测量到的TOF谱的分析比较说明：在Sq＋与H2分子碰撞实验中，库仑爆炸是产生H+的主要反应道，而氢分子离子H2+发生解离产生H+的反应道相对很弱。

高电荷态氩离子与原子碰撞中的多电子转移过程研究

本工作建立起了符合关联测量实验装置，包括反冲离子飞行时间谱仪、散射离子位置灵敏探测器、差分拉瓦型气体喷嘴、基于微机的多参数数据获取系统以及数据分析和处理程序。在入射离子能量在80KeV～240KeV范围内，利用该装置系统研究了Arq++He，Arq++Ne和Arq++Ar（q=8，9，11，12）碰撞体系中的多电子转移规律，实验鉴别了反应中发生的各种多电子转移过程，测量了反应截面，获得了一批新的实验数据。 对于Arq++He碰撞体系，本工作主要研究了He原子的转移电离相对截面与入射离子能量和电荷态的规律，发现相对截面在所研究能区基本与入射离子能量无关，并利用核间势垒和复合分子的经典图象，描述了此碰撞体系转移电离过程发生的两种可能途径，估计了相对截面的经典上限，发现在此碰撞体系中，转移电离过程中电子关联作用起着重要的作用。 本工作系统研究了Arq++He和Arq++Ar碰撞体系中多电子转移反应截面与入射离子能量、电荷态和反冲离子电荷态的变化规律，以及反冲离子电荷态分布。研究发现，在低能高电荷态离子与多电子靶原子碰撞反应中，碰撞系统的相对运动动能对碰撞体系中的电子转移过程基本没有贡献；系统所具有的势能是碰撞体系中电子转移和靶原子电离的主要因素；在相同的入射离子条件下，靶原子电离能对电子转移有重要影响；碰撞反应中单电子过程占主要地位，而在多电子转移过程中，转移电离过程发生的几率一般大于纯的多电子俘获几率；入射离子单电子俘获截面、总电荷交换截面与入射离子电荷态成正比关系；入射离子电荷交换截面随离子俘获电子数目的增加而单调减小；入射离子俘获一个电子时，转移电离截面随反冲离子电荷态的升高而单调下降，而入射离子俘获电子数多于一个时，转移电离截面存在极大值分布现象，而且分布宽度随入射离子电荷态的升高具有增加的趋势。 本工作在分析实验现象和分子经典库仑过垒模型MCBM的基础上，提出基于MCBM描述，把高电荷态离子与原子碰撞反应中的电子转移过程分为四阶段描述的新想法，即：入射过程中的分子化→复合分子形成→复合分子解离和中间态离子的形成→多电子激发态散射离子和靶离子向末态的自电离衰变。并依据能量守恒原理，规范了处理多电子激发态离子发生自电离衰变的规则。在此基础上，对Arq++He和Arq++Ar碰撞体系中的电子转移截面进行了理论计算，通过与实验结果的对比研究发现，对在中间态形成的多电子激发态散射离子，根据这些规则进行自电离衰变修正后计算得到的结果与实验符合很好，因此，对多电子激发态离子的自电离修正是合理的，而且多电子激发态离子的自电离衰变是低能高电荷态离子与原子碰撞反应中转移电离过程发生的主要因素。

The fragmentation of gold nanoparticles induced by small biomolecules

Spherical gold nanoparticles (3-5 nm) undergo a surprising fragmentation without extra energy imput and are converted into ultrasmall particles (less than 1.5 nm), which is a direct result of electron transfer between gold nanoparticles and cysteine.

Metal nanomaterials and carbon nanotubes - synthesis, functionalization and potential applications towards electrochemistry

This review focuses on the synthesis, assembly, surface functionalization, as well as application of inorganic nanostructures. Electrochemical and wet- chemical methods are demonstrated to be effective approaches to make metal nanostructures under control without addition of a reducing agent or protecting agent. Owing to the unique physical and chemical properties of the nano-sized materials, novel applications are introduced using inorganic nanomaterials, such as electrocatalysis, photoelectricity, spectrochemistry, and analytical chemistry.

Multilayer structured carbon nanotubes/poly-L-lysine/laccase composite cathode for glucose/O-2 biofuel cell

Multilayer film of laccase, poly-L-lysine (PLL) and multi-walled carbon nanotubes (MWNTs) were prepared by a layer-by-layer self-assembly technique. The results of the UV-vis spectroscopy and scanning electron microscopy studies demonstrated a uniform growth of the multilayer. The catalytic behavior of the modified electrode was investigated. The (MWNTs/PLL/laccase)(n) multilayer modified electrode catalyzed four-electron reduction of O-2 to water, without any mediator.

Magnetic control of bioelectrocatalytic processes based on assembled iron oxide particles

A facile magnetic control system was designed in bioelectrocatalytic process based on functionalized iron oxide particles. The iron oxide particles were modified with glucose oxidase, and ferrocene dicarboxylic acid was used as electron transfer mediator. Functionalized iron oxide particles can assemble along the direction of applied magnetic field, and the directional dependence of the assembled iron oxide particles can be utilized for device purposes. We report here how such functionalized magnetic particles are used to modulate the bioelectrocatalytic signal by changing the orientation of the applied magnetic field. (C) 2008 Elsevier B.V. All rights reserved.

Sensing H2O2 with layer-by-layer assembled Fe3O4-PDDA nanocomposite film

It was found that Fe3O4 nanoparticles (Fe3O4 NPs) possess intrinsic enzyme mimetic activity similar to that found in natural peroxidase. Here, we applied Fe3O4 NPs to the construction of efficient electrochemical sensor to detect the concentration of hydrogen peroxide. The sensor was fabricated with layer-by-layer assembly of Fe3O4 NPs and poly(diallyldimethylammonium chloride) (PDDA) through the electrostatic interaction, and the multilayer film was characterized with UV-vis absorption spectra, atomic force microscopy, and cyclic voltammetry.

Electrochemical characteristics of mediated laccase-catalysis and electrochemical detection of environmental pollutants

Laccase has been immobilized on the carbon nanotubes modified glassy carbon electrode surface by adsorption. As-prepared laccase retains good electrocatalytic activity to oxygen reduction by using 2,2'-azino-bis-(3-ethylbenzthiazoline-6-sulfonic acid) as the mediator. It can be used as a biosensor for the determination of catechol with broad linear range.

Properties of poly(sodium 4-styrenesulfonate)-ionic liquid composite film and its application in the determination of trace metals combined with bismuth film electrode

A new kind of bismuth film modified electrode to sensitively detect trace metal ions based on incorporating highly conductive ionic liquids 1-butyl-3-methyl-imidazolium hexafluorophosphate (BMIMPF6) in solid matrices at glassy carbon (GC) was investigated. Poly(sodium 4-styrenesulfonate) (PSS), silica, and Nafion were selected as the solid matrices. The electrochemical properties of the mixed films modified GC were evaluated. The electron transfer rate of Fe(CN)(6)(4-)/Fe(CN)(6)(3-) can be effectively improved at the PSS-BMIMPF6 modified GC.

AGET ATRP of acrylamide in aqueous media

The recently developed initiation system, the activator generated by electron transfer (AGET) was used in atom transfer radical polymerization (ATRP) to synthesize well-controlled polyacrylamide in aqueous media at 25 degrees C. The different reducing agents involved ascorbic acid and glucosa; well-controlled polymers were obtained when ascorbic acid was used as water-soluble reducing agent. The polymerizations targeted at degrees of polymerization in the range of 400 resulted in polymers with low polydispersity indices. Moreover, first order plots were linear.