Totally dressed SDCI calculations: An application to HF and F2

Summary A previously proposed procedure including the linked and unlinked contributions due to Triple and Quadruple excitations into a size-consistent SDCI-like model has been applied to HF and F₂ single-bond systems. The procedure is a non-iterative approximation to the more general total dressing model, which is based on the intermediate Hamiltonians theory. Three basis sets have been employed: the correlation consistent cc-pVTZ basis, a similar one including 3d1f polarization functions, and another including one set of g polarization functions. Excellent agreement with experiment and high-quality calculations is obtained for both equilibrium distances and spectroscopic constants. The possibilities of the method in treating single-bond breaking are also demonstrated. Finally, the Linked and Non-Linked contributions from Triple and Quadruple excitations are analysed separately and it is suggested that the addition of the linked triples to the size-consistent SDCI is sufficient to have quantitatively correct spectroscopic properties in going from the size-consistent SDCI to nearly experimental values.     

高分子结晶的新进展、新模型

回顾了高分子结晶经典模型－成核与生长模型，讨论了近年来高分子结晶研究的新结果，新进展，特别介绍了德国著名高分子物理学家Strobl提出的高分子结晶是从熔体先形成中间相，中间相转变为小晶块，最后小晶块融合为均匀为片晶的全新模型。     

Intermediate error estimates

Let R[f] be the remainder of some approximation method, having estimates of the form f;R[f]f; ρ_i ; f⁽ⁱ⁾ for i = 0,…, r. In many cases, ρ₀ and ρ_r are known, but not the intermediate error constants ρ₁,…,ρ_r−1. For periodic functions, Ligun (1973) has obtained an estimate for these intermediate error constants by ρ₀ and ρ_r. In this paper, we show that this holds in the nonperiodic case, too. For instance, the estimates obtained can be applied to the error of polynomial or spline approximation and interpolation, or to numerical integration and differentiation.     

An ant colony algorithm for the pos/neg weighted p-median problem

Let a graph G = (V, E) with vertex set V and edge set E be given. The classical graph version of the p-median problem asks for a subset of cardinality p, so that the (weighted) sum of the minimum distances from X to all other vertices in V is minimized. We consider the semi-obnoxious case, where every vertex has either a positive or a negative weight. This gives rise to two different objective functions, namely the weighted sum of the minimum distances from X to the vertices in V\X and, differently, the sum over the minimum weighted distances from X to V\X. In this paper an Ant Colony algorithm with a tabu restriction is designed for both problems. Computational results show its superiority with respect to a previously investigated variable neighborhood search and a tabu search heuristic.This research has partially been supported by the Spezialforschungsbereich F 003 “Optimierung und Kontrolle”, Projektbereich Diskrete Optimierung.     

Generalized structure of higher order nonclassicality

A generalized notion of higher order nonclassicality (in terms of higher order moments) is introduced. Under this generalized framework of higher order nonclassicality, conditions of higher order squeezing and higher order subpoissonian photon statistics are derived. A simpler form of the Hong-Mandel higher order squeezing criterion is derived under this framework by using an operator ordering theorem introduced by us in [A. Pathak, J. Phys. A 33 (2000) 5607]. It is also generalized for multi-photon Bose operators of Brandt and Greenberg. Similarly, condition for higher order subpoissonian photon statistics is derived by normal ordering of higher powers of number operator. Further, with the help of simple density matrices, it is shown that the higher order antibunching (HOA) and higher order subpoissonian photon statistics (HOSPS) are not the manifestation of the same phenomenon and consequently it is incorrect to use the condition of HOA as a test of HOSPS. It is also shown that the HOA and HOSPS may exist even in absence of the corresponding lower order phenomenon. Binomial state, nonlinear first order excited squeezed state (NLESS) and nonlinear vacuum squeezed state (NLVSS) are used as examples of quantum state and it is shown that these states may show higher order nonclassical characteristics. It is observed that the Binomial state which is always antibunched, is not always higher order squeezed and NLVSS which shows higher order squeezing does not show HOSPS and HOA. The opposite is observed in NLESS and consequently it is established that the HOSPS and HOS are two independent signatures of higher order nonclassicality.     

Intermittent dissipation and lack of universality in one-dimensional Alfvénic turbulence

The randomly driven Cohen–Kulsrud–Burgers equation is used to study the influence of viscous intermediate shocks (IS) on Alfvénic turbulence. Some of these structures are unstable and undergo gradient collapse leading, as the viscosity is reduced, to increasingly intermittent dissipation bursts. The slow decay at intermediate scales of stable IS prevents the existence of a usual inertial range. Furthermore, the dissipation is unable to adiabatically compensate for the energy injection, making the total energy sensitive to the viscosity parameter. Turbulence thus looses its universal character. Preliminary simulations extend these conclusions to magnetohydrodynamic equations with anisotropic viscosity, typical of strongly magnetized plasmas.     

Network DEA pitfalls: Divisional efficiency and frontier projection under general network structures

Data envelopment analysis (DEA) is a method for measuring the efficiency of peer decision making units (DMUs). Recently network DEA models been developed to examine the efficiency of DMUs with internal structures. The internal network structures range from a simple two-stage process to a complex system where multiple divisions are linked together with intermediate measures. In general, there are two types of network DEA models. One is developed under the standard multiplier DEA models based upon the DEA ratio efficiency, and the other under the envelopment DEA models based upon production possibility sets. While the multiplier and envelopment DEA models are dual models and equivalent under the standard DEA, such is not necessarily true for the two types of network DEA models. Pitfalls in network DEA are discussed with respect to the determination of divisional efficiency, frontier type, and projections. We point out that the envelopment-based network DEA model should be used for determining the frontier projection for inefficient DMUs while the multiplier-based network DEA model should be used for determining the divisional efficiency. Finally, we demonstrate that under general network structures, the multiplier and envelopment network DEA models are two different approaches. The divisional efficiency obtained from the multiplier network DEA model can be infeasible in the envelopment network DEA model. This indicates that these two types of network DEA models use different concepts of efficiency. We further demonstrate that the envelopment model’s divisional efficiency may actually be the overall efficiency.     

Synthesis of Sulfonimidamides from Sulfenamides via an Alkoxy‐amino‐λ6‐sulfanenitrile Intermediate

Sulfonimidamides are intriguing new motifs for medicinal and agrochemistry, and provide attractive bioisosteres for sulfonamides. However, there remain few operationally simple methods for their preparation. Here, the synthesis of NH‐sulfonimidamides is achieved directly from sulfenamides, themselves readily formed in one step from amines and disulfides. A highly chemoselective and one‐pot NH and O transfer is developed, mediated by PhIO in iPrOH, using ammonium carbamate as the NH source, and in the presence of 1 equivalent of acetic acid. A wide range of functional groups are tolerated under the developed reaction conditions, which also enables the functionalization of the antidepressants desipramine and fluoxetine and the preparation of an aza analogue of the drug probenecid. The reaction is shown to proceed via different and concurrent mechanistic pathways, including the formation of novel S≡N sulfanenitrile species as intermediates. Several alkoxy‐amino‐λ⁶‐sulfanenitriles are prepared with different alcohols, and shown to be alkylating agents to a range of nucleophiles.     

Intrinsic intermediate gap states of TiO2 materials and their roles in charge carrier kinetics

Titanium dioxide (TiO₂) is regarded as an important prototype photocatalytic material for several decades. The charge carrier kinetics determines the photocatalytic properties of TiO₂ materials; this is found to be greatly dependent on electronic structures. It has been revealed that the intrinsic intermediate gap states (intrinsic GSs) play a significant role in charge carrier kinetics that drive the photocatalytic processes of TiO₂ materials, which are not well summarized until now. Motivated by this thought, the purpose of this review focuses on physiochemical science of the intrinsic GSs of TiO₂ materials and their important role in charge carrier kinetics. We first give a summary on the chemical resources of the intrinsic GSs in TiO₂ and their physiochemical nature. Their general energy distribution, charge carrier population, and the associated thermodynamic properties are also elaborated from an overall viewpoint. We further carefully summarize and compare the experimental studies on the energy and the density distribution of the intrinsic GSs and discuss the associated chemical resources and charge carrier localizations. Trapping is the dominant function of intrinsic GSs in the charge carrier kinetics of TiO₂ materials. The significant effect of trapping on the transport, recombination, and interfacial transfer of charge carriers are also comprehensive summarized. Furthermore, the effects of charge carrier kinetics on photocatalytic performances are also discussed to some extents. Because of the importance of intrinsic GSs in modulating charge carrier kinetics, it is expected to increase the photocatalytic activity by engineering the intrinsic GSs, not only for TiO₂ materials, but also for the other semiconductor photocatalysts.     

Formation of intermediate coupling optical polarons and bipolarons in two-dimensional systems

The formation of the optical polaron and bipolaron in two-dimensional (2D) systems is studied in the intermediate electron–phonon coupling regime. The total energies of the 2D polaron and bipolaron are calculated by using the Buimistrov–Pekar method of canonical transformations. The obtained results are compared with other existing results obtained by using the Feynman path integral method and the modified Lee–Low–Pines unitary transformation method. It is shown that the electron–phonon correlation significantly reduces the total energy of the 2D polaron in comparison with the energy of the strong coupling (adiabatic) polaron. It is found that the polaron formation in 2D systems is possible when the electron–phonon coupling constant α is greater than the critical value ${\alpha }_c?2.94$, which is much lower than a critical value of the electron–phonon coupling constant α in three-dimensional (3D) systems. The critical values of the Fröhlich coupling constant α and the ratio $\eta ={\epsilon }_{\infty }/{\epsilon }_0$ (where ${\epsilon }_{\infty }$ and ${\epsilon }_0$ are the high frequency and static dielectric constants, respectively), which determine the bipolaron stability region in 2D systems, are calculated numerically. It is interesting for application to the layered cuprate superconductors that the (bi)polarons are formed more easily in quasi-2D regions than in the bulk. It is argued that the high-$T_c$ cuprate superconductivity can exist above the bulk superconducting transition temperature $T_c$ as the persisting superfluidity of polaronic (bosonic) Cooper pairs and large bipolarons at quasi-2D grain boundaries or in the CuO₂ layers above $T_c$.