硅和锗纳米线的原子排布和电荷分布的密度泛函紧束缚方法研究

低维硅锗材料是制备纳米电子器件的重要候选材料，是研发高效率、低能耗和超高速新一代纳米电子器件的基础材料之一，有着潜在的应用价值。采用密度泛函紧束缚方法分别对厚度相同、宽度在0.272 nm~0.554 nm之间的硅纳米线和宽度在0.283 nm~0.567 nm之间的锗纳米线的原子排布和电荷分布进行了计算研究。硅、锗纳米线宽度的改变使原子排布，纳米线的原子间键长和键角发生明显改变。纳米线表层结构的改变对各层内的电荷分布产生重要影响。纳米线中各原子的电荷转移量与该原子在表层内的位置相关。纳米线的尺寸和表层内原子排列结构对体系的稳定性产生重要影响。     

An adaptive multilevel wavelet framework for scale‐selective WENO reconstruction schemes

We put forth a dynamic computing framework for scale‐selective adaptation of weighted essential nonoscillatory (WENO) schemes for the simulation of hyperbolic conservation laws exhibiting strong discontinuities. A multilevel wavelet‐based multiresolution procedure, embedded in a conservative finite volume formulation, is used for a twofold purpose. (i) a dynamic grid adaptation of the solution field for redistributing grid points optimally (in some sense) according to the underlying flow structures, and (ii) a dynamic minimization of the in built artificial dissipation of WENO schemes. Taking advantage of the structure detection properties of this multiresolution algorithm, the nonlinear weights of the conventional WENO implementation are selectively modified to ensure lower dissipation in smoother areas. This modification is implemented through a linear transition from the fifth‐order upwind stencil at the coarsest regions of the adaptive grid to a fully nonlinear fifth‐order WENO scheme at areas of high irregularity. Therefore, our computing algorithm consists of a dynamic grid adaptation strategy, a scale‐selective state reconstruction, a conservative flux calculation, and a total variation diminishing Runge‐Kutta scheme for time advancement. Results are presented for canonical examples drawn from the inviscid Burgers, shallow water, Euler, and magnetohydrodynamic equations. Our findings represent a novel direction for providing a scale‐selective dissipation process without a compromise on shock capturing behavior for conservation laws, which would be a strong contender for dynamic implicit large eddy simulation approaches.     

Improved third‐order weighted essentially nonoscillatory scheme

A new third‐order WENO scheme is proposed to achieve the desired order of convergence at the critical points for scalar hyperbolic equations. A new reference smoothness indicator is introduced, which satisfies the sufficient condition on the weights for the third‐order convergence. Following the truncation error analysis, we have shown that the proposed scheme achieves the desired order accurate for smooth solutions with arbitrary number of vanishing derivatives if the parameter ε satisfies certain conditions. We have made a comparative study of the proposed scheme with the existing schemes such as WENO‐JS, WENO‐Z, and WENO‐N3 through different numerical examples. The result shows that the proposed scheme (WENO‐MN3) achieves better performance than these schemes.     

A sharp‐interface immersed boundary framework for simulations of high‐speed inviscid compressible flows

A new finite‐volume flow solver based on the hybrid Cartesian immersed boundary (IB) framework is developed for the solution of high‐speed inviscid compressible flows. The IB method adopts a sharp‐interface approach, wherein the boundary conditions are enforced on the body geometry itself. A key component of the present solver is a novel reconstruction approach, in conjunction with inverse distance weighting, to compute the solutions in the vicinity of the solid‐fluid interface. We show that proposed reconstruction leads to second‐order spatial accuracy while also ensuring that the discrete conservation errors diminish linearly with grid refinement. Investigations of supersonic and hypersonic inviscid flows over different geometries are carried out for an extensive validation of the proposed flow solver. Studies on cylinder lift‐off and shape optimisation in supersonic flows further demonstrate the efficacy of the flow solver for computations with moving and shape‐changing geometries. These studies conclusively highlight the capability of the proposed IB methodology as a promising alternative for robust and accurate computations of compressible fluid flows on nonconformal Cartesian meshes.     

Novel local smoothness indicators for improving the third‐order WENO scheme

The local smoothness indicators play an important role in the performance of a weighted essentially nonoscillatory (WENO) scheme. Due to having only 2 points available on each substencil, the local smoothness indicators calculated by conventional methods make the third‐order WENO scheme too dissipative. In this paper, we propose a different method to calculate the indicators by using all the 3 points on the global stencil of the third‐order WENO scheme. The numerical results demonstrate that the WENO scheme with the new indicators has less dissipation and better resolution than the conventional third‐order WENO scheme of Jiang and Shu for both smooth and discontinuous solutions.     

A Runge-Kutta–based WENO reconstruction on moving mesh for compressible fluids

In this paper, we construct a high-order moving mesh method based on total variation diminishing Runge-Kutta and weighted essential nonoscillatory reconstruction for compressible fluid system. Beginning with the integral form of fluid system, we get the semidiscrete system with an arbitrary mesh velocity. We use weighted essential nonoscillatory reconstruction to get the space accuracy on moving meshes, and the time accuracy is obtained by modified Runge-Kutta method; the mesh velocity is determined by moving mesh method. One- and two-dimensional numerical examples are presented to demonstrate the efficient and accurate performance of the scheme.     

A framework to perform high-order deconvolution for finite-volume method on simplicial meshes

In this article, a new framework to design high-order approximations in the context of node-centered finite volumes on simplicial meshes is proposed. The major novelty of this method is that it relies on very simple and compact differential operators, which is a critical point to achieve good performances in the High-performance computing context. This method is based on deconvolution between nodal and volume-average values, which can be conducted to any order. The interest of the new method is illustrated through three different applications: mesh-to-mesh interpolation, levelset curvature computation, and numerical scheme for convection. Higher order can also be achieved within the present framework by introducing high-rank tensors. Although these tensors feature much symmetries, their manipulation can quickly become an overwhelming task. For this reason and without loss of generality, the present articles are limited to third-order expansion. This method, although tightly connected to the k-exact schemes theory, does not rely on successive corrections: the high-order property is obtained in a single operation, which makes them more attractive in terms of performances.     

L1-type smoothness indicators based weighted essentially nonoscillatory scheme for Hamilton-Jacobi equations

This article presents an improved fifth-order finite difference weighted essentially nonoscillatory (WENO) scheme to solve Hamilton-Jacobi equations. A new type of nonlinear weights is introduced with the construction of local smoothness indicators on each local stencil that are measured with the help of generalized undivided differences in L¹-norm. A novel global smoothness measurement is also constructed with the help of local measurements from its linear combination. Numerical experiments are conducted in one- and two-dimensions to demonstrate the performance enhancement, resolution power, numerical accuracy for the proposed scheme, and compared it with the classical WENO scheme.     

d-Orbital Reconstructions Forced by Double Bow-Shaped Deformations and Second Coordination Sphere Effects of Cu(II) Heme Analogs in HER**

Both geometric architecture and electronic configurations of heme proteins contribute to its activity. In this work we designed and synthesized a series of four copper(II) porphyrin complexes ( 4 -, 3 -, 2 - and 1 -Cu) where the molecular conformations are modulated by a pair of stepwise shortened straps on the same porphyrin side (cis-ortho) to give double bow-shaped skeletons. Single crystal structures demonstrate that the straps gradually increase the saddle deformation and the deviation of the metal centers, which is in accordance with two, unusual d-orbital reconstructions of two different ground states, as revealed by 4 K EPR and DFT calculations. In the study of the electrocatalytic hydrogen evolution reaction (HER), 1 -Cu, with the shortest straps, showed the most apparent improvement of activity. Second coordination sphere (SCS) effects created by the double bow-shaped architecture and the strong saddle porphyrin core in 1 -Cu are found to play key roles in proton trapping during the catalytic process. The work contributes a novel strategy to improve the catalytic performance of heme analogs through ligand geometric modulation.     

CH4/空气简化动力学机理数值验证

选择绕圆柱预混燃烧算例，验证CH₄/空气三种简化动力学机理（16s41r、15s19r和53s325r）.考虑均匀来流，忽略湍流和湍流与燃烧相互作用以及燃料扩散效应，假设层流有限反应速率，采用保自由流5阶WENO格式求解多组分Euler方程组，得到CH₄/空气预混燃烧流场温度等值线、沿驻点线压力和温度及其CH₄、CO和CO₂质量百分数分布.结果表明：三种简化动力学机理给出的流场均出现弓形激波和火焰面，弓形激波和火焰驻点距离及其形状、诱导区宽度和简化动力学机理相关.当圆柱直径增大，弓形激波和火焰向圆柱上游移动，对应的驻点距离均增大，诱导区宽度变短，点火延时变小，但火焰和弓形激波位置次序未变化.53s325r模型要比16s41r模型和15s19r模型精度要高，点火延时覆盖的压力和温度范围也较宽，所有简化机理均未完全反应，在较大圆柱直径下游达到化学平衡.