Self-energy-functional approach to systems of correlated electrons

The grand potential of a system of interacting electrons is considered as a stationary point of a self-energy functional. It is shown that a rigorous evaluation of the functional is possible for self-energies that are representable within a certain reference system. The variational scheme allows to construct new non-perturbative and thermodynamically consistent approximations. Numerical results illustrate the practicability of the method. Received 13 January 2003 / Received in final form 5 March 2003 Published online 24 April 2003     

Photoluminescence properties of silica-based mesoporous materials similar to those of nanoscale silicon

Photoluminescence (PL) from composites of 7- and 15-nm sized silica nanoparticles (SNs) and mesoporous silicas (MSs) induced by 266- (4.66-) and 532-nm (2.33-eV) laser light has been studied at room temperature. The multiband PL from MSs in the range of 1.0-2.1 eV is evidenced to originate from isolated bulk and surface non-bridging oxygens (NBOs) and from NBOs combined with variously placed 1-nm sized pore wall oxygen vacancies (OVs). The nature and diversity of NBO light-emitters are confirmed by ab initio calculations. The PL from SNs exhibits only a short wavelength part of the bands (1.5-2.1 eV) originated from isolated bulk and surface NBOs. This fact indicates that the highly OV-bearing structures occur only in extremely thin (∼ 1 nm) silica layers. The similarity of spectroscopic properties of silica-based nanoscale materials to those of surface-oxidized silicon nanocrystals and porous silicon, containing silica-passivating layers of the same width, is discussed. Received 20 November 2000     

二甲苯在ZSM-5分子筛中的吸附与扩散

本文在298K-493K温度范围内,测定了二甲苯在ZSM-5分子筛中的吸附等温线和扩散系数。间二甲苯在HZSM-5分子筛中的吸附是需要较高活化能而为扩散控制的物理吸附,只有在较高温度下(>393K),才能进入分子筛的敛孔,其扩散系数比对二甲苯小三个数量级。对、间二甲苯在HZSM-5分子筛中的吸附量随温度升高而渐趋接近。但HZSM-5经镁改性后,间二甲苯吸附量大幅度下降,而对二甲苯吸附量变化不大,说明孔道结构因素对提高烷基苯转化的对位选择性起着相当重要的作用。增大分子筛的晶粒尺寸,二甲苯的扩散系数变化不大,表明大晶粒ZSM-5之所以能提高对位选择性,原因在于扩散路线的增长导致扩散较慢的间二甲苯异构化为扩散较快的对二甲苯。     

Sputtering yields for light ions as a function of angle of incidence

The sputtering yield of Ni, Mo, and Au have been measured at oblique angles of incidence for H⁺-, D⁺-, and⁴He⁺-ion irradiation in the energy region from 1 to 8 keV. The yields were determined from the weight loss of the targets. For Ni and Mo the dependence of the sputtering yield on the angle of incidence was found to be much stronger for H⁺- and D⁺-ion than for⁴He⁺-ion irradiation. In all cases the maximum in the yield was found at angles of incidence ϑ≧80°, where ϑ is the angle measured from the surface normal. Furthermore the ratio of the maximum yield to the yeild at normal incidence increases with increasing surface binding energy of the target material as well as with increasing ion energy in the energy region inveestigated. The results are discussed qualitatively in view of a model for the sputtering mechanism for light ions.     

Azimuthal anchoring of liquid crystals at the surface of photo-induced anisotropic films

Received: 13 November 1996/Accepted: 22 January 1997     

Light-matter interactions within the Ehrenfest–Maxwell–Pauli–Kohn–Sham framework: fundamentals,implementation, and nano-optical applications

In recent years significant experimental advances in nano-scale fabrication techniques and in available light sources have opened the possibility to study a vast set of novel light-matter interaction scenarios, including strong coupling cases. In many situations nowadays, classical electromagnetic modeling is insufficient as quantum effects, both in matter and light, start to play an important role. Instead, a fully self-consistent and microscopic coupling of light and matter becomes necessary. We provide here a critical review of current approaches for electromagnetic modeling, highlighting their limitations. We show how to overcome these limitations by introducing the theoretical foundations and the implementation details of a density-functional approach for coupled photons, electrons, and effective nuclei in non-relativistic quantum electrodynamics. Starting point of the formalism is a generalization of the Pauli–Fierz field theory for which we establish a one-to-one correspondence between external fields and internal variables. Based on this correspondence, we introduce a Kohn-Sham construction which provides a computationally feasible approach for ab-initio light-matter interactions. In the mean-field limit, the formalism reduces to coupled Ehrenfest–Maxwell–Pauli–Kohn–Sham equations. We present an implementation of the approach in the real-space real-time code Octopus using the Riemann–Silberstein formulation of classical electrodynamics to rewrite Maxwell's equations in Schrödinger form. This allows us to use existing very efficient time-evolution algorithms developed for quantum-mechanical systems also for Maxwell's equations. We show how to couple the time-evolution of the electromagnetic fields self-consistently with the quantum time-evolution of the electrons and nuclei. This approach is ideally suited for applications in nano-optics, nano-plasmonics, (photo) electrocatalysis, light-matter coupling in 2D materials, cases where laser pulses carry orbital angular momentum, or light-tailored chemical reactions in optical cavities just to name but a few.     

Formability and Thermal Stability of Ce62Al15Fe8Co15 Bulk Metallic Glass

The formability and thermal stability of Ce62Al15Fe8Co15 bulk metallic glass （BMG） are studied by x-ray diffraction （XRD） and differential scanning calorimetry. The critical diameter of Ce62Al15Fe8Co15 BMG predicted by the parameter γ is about 3.1 mm, which is roughly in agreement with the XRD results. Stability of the BMG is investigated by means of continuous crystallization diagrams obtained from the extension of the Kissinger and Vogel-Fulcher-Tammann （VFT） equations comparatively. It is found that the dependence of crystallization temperature of the BMG on heating rates follows a nonlinear relationship rather than Kissinger and Lasoka＇s linear fittings. The thermal stability of the BMG is investigated by the VFT equation.     

Clockwise vs Counter-Clockwise I-V Hysteresis of Point-Contact Metal-Tip/Pr0.7 Ca0.3MnO3/Pt Devices

Metal-tip/Pr0.7Ca0.3MnO3/Pt devices possess two types of I-V hysteresis： clockwise vs counter clockwise depending on the tip materials. The criteria for categorization of these two types of devices can be simply based on whether the Gibbs free energy of oxidation for the metal tip is lower or higher than that of PCMO, respectively. While the clockwise hysteresis can be attributed to electric field induced oxidation/reduction, the counter clockwise hysteresis can be explained by oxygen vacancy migration in an electrical field. Alternating-current conductance spectra also reveal distinct hopping barriers between these two categories of devices at high resistive states.