Coulomb asymmetry in strong field multielectron ionization of diatomic molecules

We measure the angular distribution of an electron emitted by a strong elliptically polarized two-color laser field from exploding doubly charged molecular nitrogen. This angular distribution is vastly different for emission of the electron from the up-field core of the molecule as compared to that from the down-field core. The emission from the down-field core leads to a slight rotation with respect to the internuclear axis in the direction expected by the Coulomb effect of the remaining ion, while, for the emission from the up-field core, this direction is inversed. Our semiclassical simulations suggest that this unexpected angular distribution is caused by an initial longitudinal momentum of the electron freed by over-the-barrier ionization above the inner barrier in the molecule. The initial kinetic energy is in the range of the potential energy of the Stark-shifted orbital above the barrier.     

An acousto-optical imaging spectrometer for astrophysical measurements

An optical scheme of an acousto-optical imaging spectrometer for observing extended astrophysical objects with line emission spectra is proposed. The use of an additional prism with a specified angular dispersion makes it possible to separate images of an extended object at different emission lines and images generated by minor maxima of the acousto-optical filter transmission function. A prototype of the imaging spectrometer has been designed.     

Ionization of diatomic molecules by electron impact

An analytical expression for the amplitude of ionization of the hydrogen molecule by electron impact in the first Born approximation with a one-center Coulomb continuum wave function is derived. The case where the incident electron energy is much greater than the ejected electron energy is considered. The molecular wave functions were constructed in the approximation of linear combination of atomic orbitals with overlapping configurations. The role of the orthogonalization of the initial and final wave functions of the active electron of the target is elucidated. The triple differential ionization cross sections for the different orientations of the molecular axis and that averaged over all orientations are calculated. The secondary electron angular distribution is represented in the form of three-dimensional images. A comparison with the results of other theoretical calculations and experimental data is performed.     

Double photoionization of rotating linear molecules

This communication presents a theoretical study of the angular distribution of one or both of the two electrons emitted in one-photon, one-step double ionization of a linear molecule. Experiments which do or do not detect spin of the photoelectrons have been considered. Effects of molecular rotation on double photoionization have been studied in both Hund's coupling schemes (a) and (b) by using parity-adapted states. Selection rules obtained in this paper are very different from those derived earlier for single photoionization and for Auger decay following the absorption of a photon in a rotating linear molecule. It is shown that complete specification of the spin-unresolved and of spin-resolved angular distributions of both photoelectrons require, respectively, three and seven parameters which depend, among other things, on their energies as well as directions of emission. The approach developed in this paper has been used to analyze spin-unresolved double photoionization in the shell of the molecule. The angular distribution is quite different depending on whether or not molecular rotation has been taken into account. Also, it is found to change significantly for different rotational transitions. Effects of electron-electron correlation are clearly manifested even in non-coincident, both rotationally resolved--as well as unresolved--double photoionization. Received: 7 August 1998     

Resonant-cavity light-emitting diodes: quantum noise and spatial emission characteristics

We demonstrate the interplay between the intensity noise and the spatial emission characteristics of resonant-cavity light-emitting diodes. First, we find that the total aperture intensity noise exhibits a sub-shot noise behavior in a quite large pumping regime. Second, we investigate the angular, spectral, and spatial emission characteristics of the devices by controlling the shape and width of the angular intensity distribution via temperature detuning of the quantum well wavelength and the cavity resonance wavelength. Finally, the angular and aperture resolved intensity noise exhibit a super-shot noise behavior in contrast to that of the total emission. We explain this difference with anticorrelations between various radial components which increase with the temperature-tuned extension of the spatial emission. PACS 85.60.Jb; 42.50.L; 23.20.En     

Fluorescence characteristics of a molecule in the vicinity of a plasmonic nanomatryoska: Nonlocal optical effects

The fluorescence characteristics of a dipole molecule in the vicinity of a spherical multilayered metallic nanoshell (a plasmonic nanomatryoska) of ultra-small dimensions is studied via electrodynamic modeling, where we have computed the fluorescence decay rates, the shifts in emission frequency, and the overall fluorescence yields for molecular dipoles of both tangential and radial orientations. Our focus is on structures of ultra small dimensions in order to elucidate the possibly novel nonlocal optical effects in such a phenomenon. The results show that at very close distances between the molecule and the nanoshell, the nonlocal effects in general lead to smaller structure-induced effects with broadened and blue-shifted plasmonic resonances. These effects include overall smaller induced decay rates, smaller red-shifts in emission frequency, and somewhat larger fluorescence yields at low emission frequencies. Physical interpretation of our simulation results is provided.     

Circularly polarized unidirectional emission via a coupled plasmonic spiral antenna

In this Letter, we study the emission properties of an electric dipole emitter coupled to a plasmonic spiral structure. The plasmonic spiral structure functions as an optical antenna, coupling the electric dipole emission into circularly polarized unidirectional emission in the far field. Increasing number of turns of the spiral leads to narrower angular width of the emission pattern in the far field. For a spiral antenna with six turns, antenna directivity of 23.5 dB with a directional emission into a narrow angular cone of 4.3° can be achieved. The emitted photons carry spin that is essentially determined by the handedness of the spiral antenna. By reversing the spiral, one can switch the polarization of the emission field between left-hand and right-hand circular polarizations. The spiral antenna may be used as a nanoscale circular polarization source in single molecule sensing, single-photo sources, and integrated photonic circuits.     

一种共轭聚合物单分子发色团吸收和发射特性动态演变过程的实时测量

利用频域信息重构的散焦宽场成像测量了Poly[2,7-(9,9-dioctylfluorene)-alt-4,7-bis(thiophen-2-yl)benzo-2,1,3-thiadiazole](PFO-DBT)共轭聚合物单分子发色团的吸收与发射特性及其动态演变过程.通过调制用于激发共轭聚合物单分子的超短脉冲对的相对相位,对单分子荧光进行傅里叶变换的频域测量,跟踪发色团吸收偶极取向变化;通过测量散焦荧光成像光斑探测发色团发射偶极取向变化.研究发现, PFO-DBT共轭聚合物单分子发色团存在吸收和发射偶极取向均保持不变、其中之一变化以及两者同时变化三种情况.这种对共轭聚合物单分子发色团吸收和发射偶极取向演化过程的实时测量可用于分析共轭聚合物构象变化及其对能量转移过程的影响.     

Interferences from fast electron emission in molecular photoionization

We present a theoretical study of fast-electron emission produced in H2 and H2+ photoionization. We show that, when the electron wave length is comparable to the molecular size, the electron angular distributions arising from fixed-in-space molecules exhibit pronounced interference effects that critically depend on orientation and energy sharing between electrons and nuclei. In particular, for molecules oriented parallel to the polarization direction, the angular patterns reveal a complex nodal structure, while for molecules oriented perpendicularly, typical Young's double-slit interferences are observed. These patterns change dramatically as the molecule vibrates.     

Angular distributions of H2 desorbed from the (100), (110), and (111) faces of copper crystals

The angular distributions of hydrogen molecules desorbed from copper have been measured for single-crystal surfaces of three different orientations: (100), (110), and (111). The surfaces were cleaned to the degree that the impurities were below the level of detection by Auger electron spectroscopy. The angular distributions were all significantly more peaked at the surface normal than the distribution corresponding to diffuse emission, i.e., where the molecular flux is proportional to cos θ, where θ is the angle measured from the surface normal. We have characterized the observed angular distributions by fitting the emperical expression cos^dθ to the data, where d is an adjustable parameter. The results are: d ≈ 5 for (100); d ≈ 2.5 for (110); d ≈ 6 for (111). The distributions are nearly symmetric about the azimuthal angle between the plane of detection and the principal axes of the surface lattice. Possible models are considered.     

Lattice Boltzmann Simulation of Sedimentation of a Single Elastic Dumbbell in a Newtonian Fluid

Based on the lattice Boltzmann method (LBM), the sedimentations of a single elastic dumbbell in a Newtonian fluid under different initial positions and orientations, and also that of the elastic dumbbells with different free lengths of the spring under the same initial conditions have been simulated. All of the numerical results show that the final orientations of the elastic dumbbells are in the same horizontal direction, and the final positions of their centroids are all on the centerline of the tube no matter what the initial positions and orientations of the elastic dumbbell or the free lengths of the spring are. When the elastic dumbbell finally falls down vertically, the two circular cylinders of the elastic dumbbell rotate around their own symmetry-axis respectively, and their angular velocities are equal but opposite to each other. For the sedimentations of the elastic dumbbells with different free lengths of the spring, the shorter of the free length is, the faster the final angular velocity and vertical velocity of the circular cylinder will be.     

同位旋对断前粒子发射影响的角动量依赖性

对一个同量异位素链²⁰²Fr,²⁰²Po,²⁰²Tl和一个同位素链^189,202,212Po,用裂变扩散模型考察了角动量对裂变前粒子发射同位旋效应的影响.发现断前粒子发射的同位旋效应敏感地依赖于系统的自旋.高的角动量不但弱化了同位旋对粒子蒸发的影响,而且也降低了核耗散对粒子发射的影响.因此,为了更准确地用粒子多重性来提取核耗散系数,选择一个低自旋的复合系统是重要的     

Measurement of the magnetomechanical effect in a gas discharge

The centrifugal dipole moments of the methane molecule are numerically calculated and their behavior at large quantum numbers of the total angular momentum of the molecule are analyzed.     

Experimentally observed orientation of C60F18 molecules on the nickel single crystal (100) surface

The angular dependence of near edge X-ray absorption fine structure (NEXAFS) spectra has been obtained in the vicinity of carbon and fluorine 1s absorption edges in a monolayer film of polar fullerene fluoride (C₆₀F₁₈) molecules on a Ni(100) substrate. The fine structure of the spectra has been identified according to experimental data via calculations based on the density functional theory, and the angular dependence of the spectra has been explained. The orientations of structural molecular fragments are determined from the angular dependence of the NEXAFS spectra. It is demonstrated that the electric dipole moment of a C₆₀F₁₈ molecule is oriented along the normal to the substrate surface with an accuracy of 5°.     

Lattice Boltzmann Simulation of Sedimentation of a Single Elastic Dumbbell in a Newtonian Fluid

Based on the lattice Boltzmann method (LBM), the sedimentations of a single elastic dumbbell in a Newtonian fluid under different initial positions and orientations, and also that of the elastic dumbbells with different free lengths of the spring under the same initial conditions have been simulated. All of the numerical results show that the final orientations of the elastic dumbbells are in the same horizontal direction, and the final positions of their centroids are all on the centerline of the tube no matter what the initial positions and orientations of the elastic dumbbell or the free lengths of the spring are. When the elastic dumbbell finally falls down vertically, the two circular cylinders of the elastic dumbbell rotate around their own symmetry-axis respectively, and their angular velocities are equal but opposite to each other. For the sedimentations of the elastic dumbbells with different free lengths of the spring, the shorter of the free length is, the faster the final angular velocity and vertical velocity of the circular cylinder will be.     

线型分子的电子能级之Λ分裂的新解释

认为电子态能级发生Λ分裂虽然是角动量引起的,但不是耦合而是运动牵连作用的结果.从这一认识出发,利用欧拉方程和拉格朗日方程分别得到了包含Λ分裂的分子转动哈密顿函数和哈密顿算符,所得结果与Van.Vleck的著名结论完全一致 关键词： Λ分裂 线型分子 欧拉方程 哈密顿算符     

Preferred orientations of encapsulated C60 molecules inside single wall carbon nanotubes

A systematical study of the orientational behavior of C60 molecules in single wall carbon nanotubes (SWCNTs) with different chirality and diameter has been performed by using a model of an infinite long nanotube filled with two C60 (denoted as C60-1 and C60-2) molecules. We studied the preferred orientation of the C60-1 molecule when the neighboring C60-2 molecule was fixed at the pentagon, double-bond, and hexagon orientations respectively. Our results showed that the C60-1 molecule prefers the pentagon (hexagon) orientation when the tube diameter is smaller (larger) than 1.31nm (1.36nm). For the tube diameter in between, the preferred molecular orientation of C60-1 changes from pentagon to hexagon with the increasing tube diameter when the neighboring C60-2 molecule is fixed at the pentagon or double-bond orientation. A novel vertex orientation for the C60-1 molecule has been found when the C60-2 molecule is fixed at the hexagon orientation.     

Angular distributions of electrons photoemitted from chemisorbed atoms

A theory which describes the angular distributions of electrons photo-emitted from chemisorbed atoms is presented. Due to hole delocalization and preferential orientation, interference effects due to emission from various centers in a molecule do not average out, as they do in gas phase photoionization and much more structural information pertaining to chemisorption bonds is contained in such measurements.     

Optical nuclear polarization for sensitivity enhancement of2H NMR single-crystal studies

A gain in detection sensitivity of more than three orders of magnitude is achieved in high-resolution solid-state²H nuclear magnetic resonance of monocrystalline fluorene-d₁₀ by applying optical nuclear polarization via excited triplet states of acridine-h₉ guest molecules. The sensitivity gain is utilized to measure the angular dependence (rotation pattern) of the²H nuclear magnetic resonance lines. In this way the principal values and orientations of all²H quadrupolar tensors are determined. Except for the methylene deuterons, all tensors belonging to the same molecule have one principal axis in common, namely the axis perpendicular to the molecular plane, showing that in the crystal lattice the fluorene molecule is in a planar configuration.