飞秒强激光作用下电子振荡导致的谐波辐射频谱的展宽和红移

采用单电子模型研究了圆偏振飞秒脉冲激光作用下电子振荡导致的谐波辐射频谱的特性。研究发现随着激光强度的增加，电子在激光场中运动的相对论效应可以导致谐波辐射，并且发现谐波辐射频谱随着激光强度的增加发生了展宽和红移。电子与强激光脉冲相互作用，电子除了在激光场的作用下做横向振荡运动之外，激光脉冲的纵向有质动力对电子还有推动作用，这是产生谐波频谱红移的原因，而谐波辐射频谱展宽是由电子纵向速度的变化引起的。分析激光场中电子在不同方向的辐射频谱表明：随着谐波阶数的升高，红移在有规律地变大；在θ=3π／4方向上电子频谱的

Design, Synthesis, and Study of Novel Platforms for Iron-N2 Chemistry and Photoinduced, Copper-mediated C-N Bond Formation

Several new ligand platforms designed to support iron dinitrogen chemistry have been developed. First, we report Fe complexes of a tris(phosphino)alkyl (CP^iPr₃) ligand featuring an axial carbon donor intended to conceptually model the interstitial carbide atom of the nitrogenase iron-molybdenum cofactor (FeMoco). It is established that in this scaffold, the iron center binds dinitrogen trans to the C_alkyl anchor in three structurally characterized oxidation states. Fe-C_alkyl lengthening is observed upon reduction, reflective of significant ionic character in the Fe-C_alkyl interaction. The anionic (CP^iPr₃)FeN₂^- species can be functionalized by a silyl electrophile to generate (CP^iPr₃)Fe-N₂SiR₃. This species also functions as a modest catalyst for the reduction of N₂ to NH₃. Next, we introduce a new binucleating ligand scaffold that supports an Fe(μ-SAr)Fe diiron subunit that coordinates dinitrogen (N₂-Fe(μ-SAr)Fe-N₂) across at least three oxidation states (Fe^IIFe^II, Fe^IIFe^I, and Fe^IFe^I). Despite the sulfur-rich coordination environment of iron in FeMoco, synthetic examples of transition metal model complexes that bind N₂ and also feature sulfur donor ligands remain scarce; these complexes thus represent an unusual series of low-valent diiron complexes featuring thiolate and dinitrogen ligands. The (N₂-Fe(μ-SAr)Fe-N₂) system undergoes reduction of the bound N₂ to produce NH₃ (~50% yield) and can efficiently catalyze the disproportionation of N₂H₄ to NH₃ and N₂. The present scaffold also supports dinitrogen binding concomitant with hydride as a co-ligand. Next, inspired by the importance of secondary-sphere interactions in many metalloenzymes, we present complexes of iron in two new ligand scaffolds ([SiP^NMe₃] and [SiP^iPr₂P^NMe]) that incorporate hydrogen-bond acceptors (tertiary amines) which engage in interactions with nitrogenous substrates bound to the iron center (NH₃ and N₂H₄). Cation binding is also facilitated in anionic Fe(0)-N₂ complexes. While Fe-N₂ complexes of a related ligand ([SiP^iPr₃]) lacking hydrogen-bond acceptors produce a substantial amount of ammonia when treated with acid and reductant, the presence of the pendant amines instead facilitates the formation of metal hydride species.

Additionally, we present the development and mechanistic study of copper-mediated and copper-catalyzed photoinduced C-N bond forming reactions. Irradiation of a copper-amido complex, ((m-tol)₃P)₂Cu(carbazolide), in the presence of aryl halides furnishes N-phenylcarbazole under mild conditions. The mechanism likely proceeds via single-electron transfer from an excited state of the copper complex to the aryl halide, generating an aryl radical. An array of experimental data are consistent with a radical intermediate, including a cyclization/stereochemical investigation and a reactivity study, providing the first substantial experimental support for the viability of a radical pathway for Ullmann C-N bond formation. The copper complex can also be used as a precatalyst for Ullmann C-N couplings. We also disclose further study of catalytic C_alkyl-N couplings using a CuI precatalyst, and discuss the likely role of [Cu(carbazolide)₂]^- and [Cu(carbazolide)₃]^- species as intermediates in these reactions.

Finally, we report a series of four-coordinate, pseudotetrahedral P₃Fe^II-X complexes supported by tris(phosphine)borate ([PhBP₃Fe^R]^-) and phosphiniminato X-type ligands (-N=PR'₃) that in combination tune the spin-crossover behavior of the system. Low-coordinate transition metal complexes such as these that undergo reversible spin-crossover remain rare, and the spin equilibria of these systems have been studied in detail by a suite of spectroscopic techniques.

Electronic structure in GaAs/AlxGa1-xAs spherical quantum dots

In this paper, how the dots' radius, At concentration and external electric field affect the single electron energy states in GaAs/AlxGa1-xAs spherical quantum dots are discussed in detail. Furthermore, the modification of the energy states is calculated when the difference in effective electron mass in GaAs and AlxGa1-xAs are considered. In addition, both the analytical method and the plane wave method are used in calculation and the results are compared, showing that they are in good agreement with each other. The results and methods can provide useful information for the future research and potential applications of quantum dots.

Compact universal logic gates realized using quantization of current in nanodevices

This paper proposes novel universal logic gates using the current quantization characteristics of nanodevices. In nanodevices like the electron waveguide (EW) and single-electron (SE) turnstile, the channel current is a staircase quantized function of its control voltage. We use this unique characteristic to compactly realize Boolean functions. First we present the concept of the periodic-threshold threshold logic gate (PTTG), and we build a compact PTTG using EW and SE turnstiles. We show that an arbitrary three-input Boolean function can be realized with a single PTTG, and an arbitrary four-input Boolean function can be realized by using two PTTGs. We then use one PTTG to build a universal programmable two-input logic gate which can be used to realize all two-input Boolean functions. We also build a programmable three-input logic gate by using one PTTG. Compared with linear threshold logic gates, with the PTTG one can build digital circuits more compactly. The proposed PTTGs are promising for future smart nanoscale digital system use.

Weak measurement of qubit oscillations with strong response detectors: Violation of the fundamental bound imposed on linear detectors

Qubit measurement by mesoscopic charge detectors has received great interest in the community of mesoscopic transport and solid-state quantum computation, and some controversial issues still remain unresolved. In this work, we revisit the continuous weak measurement of a solid-state qubit by single electron transistors (SETs) in nonlinear-response regime. For two SET models typically used in the literature, we find that the signal-to-noise ratio can violate the universal upper bound "4," which is imposed quantum mechanically on linear-response detectors. This different result can be understood by means of the cross correlation of the detector currents by viewing the two junctions of the single SET as two detectors. Possible limitation of the potential-scattering approach to this result is also discussed.

Electronic transport through self-assembled quantum disks

In this paper we study a single electron tunneling through a vertically stacked self-assembled quantum disks structure using a transfer matrix technique in the framework of effective mass approximation. In the disks, the electron is confined both laterally and vertically; we separate the motion in the vertical and lateral directions within the adiabatic approximation and treat the energy levels of the latter as an effective confining potential. The influence of a constant applied electric field is taken into account using an exact Airy-function formalism and the current density is calculated at zero temperature. By increasing the widths of the barriers, we find the peaks of the current density shift toward lower voltage region; meanwhile, they can become even sharper. (C) 2004 Elsevier Ltd. All rights reserved.

Influence of level filling on optical properties of quantum well

In a specially- designed three-barrier-double-well tunneling structure, electron injecting from the emitter in combination with escaping through a resonant-tunneling structure were used to adjust and control the filling of electrons in different subbands. It was observed that the occupation in the first-excited electron state can result in a suppression to quantum confinement Stark effect. Moreover, at very low bias, a series of intrigue photoluminescence peaks appeared as a small quantity of excess electron was filled in the ground state of the quantum well, that cannot be explained by the theory of hand-to-hand transition in the framework of single electron picture.

Electronic structures of GaAs/AlxGa1-xAs quantum double

In the framework of effective mass envelope function theory, the electronic structures of GaAs/AlxGa1-xAs quantum double rings(QDRs) are studied. Our model can be used to calculate the electronic structures of quantum wells, wires, dots, and the single ring. In calculations, the effects due to the different effective masses of electrons and holes in GaAs and AlxGa1-xAs and the valence band mixing are considered. The energy levels of electrons and holes are calculated for different shapes of QDRs. The calculated results are useful in designing and fabricating the interrelated photoelectric devices. The single electron states presented here are useful for the study of the electron correlations and the effects of magnetic fields in QDRs.

Analog computation using quantum-dot cell network

A novel analog-computation system using a quantum-dot cell network is proposed to solve complex problems. Analog computation is a promising method for solving a mathematical problem by using a physical system analogous to the problem. We designed a novel quantum-dot cell consisting of three-stacked. quantum dots and constructed a cell network utilizing the nearest-neighbor interactions between the cells. We then mapped a graph 3-colorability problem onto the network so that the single-electron configuration of the network in the ground state corresponded to one of the solutions. We calculated the ground state of the cell network and found solutions to the problems. The results demonstrate that analog computation is a promising approach for solving complex problems.

Electronic states of InAs/GaAs quantum ring

In the framework of effective mass envelope function theory, the electronic states of the InAs/GaAs quantum ring are studied. Our model can be used to calculate the electronic states of quantum wells, quantum wires, and quantum dots. In calculations, the effects due to the different effective masses of electrons in rings and out rings are included. The energy levels of the electron are calculated in the different shapes of rings. The results indicate that the inner radius of rings sensitively changes the electronic states. The energy levels of the electron are not sensitively dependent on the outer radius for large rings. If decreasing the inner and outer radii simultaneously, one may increase the energy spacing between energy levels and keep the ground state energy level unchanged. If changing one of two radii (inner or outer radius), the ground state energy level and the energy spacing will change simultaneously. These results are useful for designing and fabricating the double colors detector by intraband and interband translations. The single electron states are useful for studying the electron correlations and the effects of magnetic fields in quantum rings. Our calculated results are consistent with the recent experimental data of nanoscopic semiconductor rings. (C) 2001 American Institute of Physics.

Self-assembled GaAs quantum rings by MBE droplet epitaxy

Fabrication of semiconductor nanostructures such as quantum dots (QDs), quantum rings (QRs) has been considered as the important step for realization of solid state quantum information devices, including QDs single photon emission source, QRs single electron memory unit, etc. To fabricate GaAs quantum rings, we use Molecular Beam Epitaxy (MBE) droplet technique in this report. In this droplet technique, Gallium (Ga) molecular beams are supplied initially without Arsenic (As) ambience, forming droplet-like nano-clusters of Ga atoms on the substrate, then the Arsenic beams are supplied to crystallize the Ga droplets into GaAs crystals. Because the morphologies and dimensions of the GaAs crystal are governed by the interplay between the surface migration of Ga and As adatoms and their crystallization, the shape of the GaAs crystals can be modified into rings, and the size and density can be controlled by varying the growth temperatures and As/Ga flux beam equivalent pressures(BEPs). It has been shown by Atomic force microscope (AFM) measurements that GaAs single rings, concentric double rings and coupled double rings are grown successfully at typical growth temperatures of 200 C to 300 C under As flux (BEP) of about 1.0 x 10(-6) Torr. The diameter of GaAs rings is about 30-50 nm and thickness several nm.

TUNNELING ESCAPE TIME OF ELECTRONS THROUGH DOUBLE-BARRIER RESONANT-TUNNELING STRUCTURES

Tunneling escape of electrons from quantum wells (QWs) has systematically been studied in an arbitrarily multilayered heterostructures, both theoretically and experimentally. A wave packet method is developed to calculate the bias dependence of tunneling escape time (TET) in a three-barrier, two-well structure. Moreover, by considering the time variation of the band-edge profile in the escape transient, arising from the decay of injected electrons in QWs, we demonstrate that the actual escape time of certain amount of charge from QWs, instead of single electron, could be much longer than that for a single electron, say, by two orders of magnitude at resonance. The broadening of resonance may also be expected from the same mechanism before invoking various inhomogeneous and homogeneous broadening. To perform a close comparison between theory and experiment, we have developed a new method to measure TET by monitoring transient current response (TCR), stemming from tunneling escape of electrons out of QWs in a similar heterostructure. The time resolution achieved by this new method reaches to several tens ns, nearly three orders of magnitude faster than that by previous transient-capacitance spectroscopy (TCS). The measured TET shows an U-shaped, nonmonotonic dependence on bias, unambiguously indicating resonant tunneling escape of electrons from an emitter well through the DBRTS in the down-stream direction. The minimum value of TET obtained at resonance is accordance with charging effect and its time variation of injected electrons. A close comparison with the theory has been made to imply that the dynamic build-up of electrons in DBRTS might play an important role for a greatly suppressed tunneling escape rate in the vicinity of resonance.

STUDIES ON TUNNELING ESCAPE TIME OF ELECTRONS FROM A QUANTUM-WELL IN MULTILAYERED HETEROSTRUCTURES

By considering the time variation of band-edge profile arising from the decay of injected charge in quantum wells(QWs), we employ a wave packet method to verify that the actual escape time of certain amount of electrons from QWs could be much larger than that for a single electron. The theoretical result is also in agreement with our measurement of escape time, performed by using a newly developed method--transient current response.

Quantum computation using artificial molecules

Two kinds of quantum computation systems using artificial molecules: quantum computer and quantum analog computer are described. The artificial molecule consists of two or three coupled quantum dots stacked along z direction and one single electron, In quantum computer, one-qubit and two-qubit gates are constructed by one molecule and two molecules, respectively. The coupling between two qubits in a quantum gate can be controlled by thin film electrodes. We also constructed a quantum analog computer by designing a three-dot molecule network and mapping a graph 3-colorability problem onto the network. The ground-state configuration of the single electrons in the network corresponds to one of the problem solutions, We numerically study the operations of the two kinds of the quantum computers and demonstrate that they quantum gates can perform the quantum computation and solve complex problems.

Analog computation using quantum-dot cell network

A novel analog-computation system using a quantum-dot cell network is proposed to solve complex problems. Analog computation is a promising method for solving a mathematical problem by using a physical system analogous to the problem. We designed a novel quantum-dot cell consisting of three-stacked. quantum dots and constructed a cell network utilizing the nearest-neighbor interactions between the cells. We then mapped a graph 3-colorability problem onto the network so that the single-electron configuration of the network in the ground state corresponded to one of the solutions. We calculated the ground state of the cell network and found solutions to the problems. The results demonstrate that analog computation is a promising approach for solving complex problems.