Nuclear forward scattering vs. conventional Mössbauer studies of atomically tailored Eu-based materials

With the decrease in size of devices, rapid characterization of nano-devices is an inevitable necessity. It is shown that Mössbauer spectroscopy using synchrotron radiation from the advanced photon source provides such a tool of investigation. Results are presented and compared for conventional Mössbauer and Nuclear Forward Scattering for ¹⁵¹Eu-doped magnesium sulfide as an example, especially at low concentrations.     

Tailoring approach for exploring electron densities and electrostatic potentials of molecular crystals

Experimental and theoretical studies of electron densities and the corresponding derived entities such as electrostatic potentials have been the primary means of understanding the chemical nature and electronic properties of crystalline substances. Conventional crystal calculation methods such as the embedded cluster models are capable of performing calculations on small and medium-sized molecules, while periodic ab initio methods can treat crystals with up to 200 atoms per unit cell. A linear scaling method, viz. the molecular tailoring approach, has recently been developed for obtaining ab initio quality one-electron properties. In the present study, the molecular tailoring approach is employed to generate electron density, electrostatic potential and interaction density maps with the ibuprofen crystal as a test case. The interaction density and electrostatic potential maps produced in the present work succinctly bring out the actual crystalline environment around a given reference molecule by including the interactions with atoms in its neighborhood. The results obtained from the molecular tailoring approach may thus be expected to enhance our understanding of the environment in the crystalline material with reasonably small computational effort.Contribution to the Jacopo Tomasi Honorary Issue     

Morphology-controlled electrochemical sensing amaranth at nanomolar levels using alumina

Different-shaped aluminas were readily prepared via hydrothermal reaction. It was found that the morphology and the electrochemical sensing properties of alumina were heavily dependent on the reaction time. When extending the reaction time from 6 h to 24 h, the obtained alumina samples changed from amorphous bumps to regular microfibers in diameter of 200 nm, as confirmed by scanning electron microscopy. Transmission electron microscopy observation revealed that longer reaction time was beneficial for the formation of porous and uniform fiber-like structures. Electrochemical tests proved that alumina microfibers were more active for the oxidation of amaranth and exhibited much higher enhancement effect, compared with alumina bumps. On the surface of alumina microfibers, the oxidation peak currents of amaranth increased remarkably. The influences of pH value, amount of alumina microfibers, and accumulation time on the signal enhancement of amaranth were discussed. As a result, a novel electrochemical method was developed for the detection of amaranth. The linear range was from 1 to 150 nM, and the detection limit was 0.75 nM after 1-min accumulation. The analytical application in drink samples was investigated, and the results consisted with the values that obtained by high-performance liquid chromatography.     

Selective switching of individual multipole resonances in single dielectric nanoparticles

Following Mie theory, nanoparticles made of a high‐refractive‐index dielectric, such as silicon, exhibit a resonator‐like behavior and very rich resonance spectra. Which electric or magnetic particle mode is excited depends on the wavelength, the refractive‐index contrast relative to the environment, and the geometry of the nanoparticle itself. In addition, the spatial structure of the impinging light field plays a major role in the excitation of the nanoparticle resonances. Here, it is shown that, by tailoring the excitation field, individual multipole resonances can be selectively addressed while suppressing the excitation of other particle modes. This enables a detailed study of selected individual resonances without interference by the other modes.

     

Quantitative decomposition of resonance-assisted hydrogen bond energy in β-diketones into resonance and hydrogen bonding (π- and σ-) components using molecular tailoring and function-based approaches

Using the molecular tailoring and function-based approaches allows one to divide the energy of the O─H⋯O═C resonance-assisted hydrogen bond in a series of the β-diketones into resonance and hydrogen bonding components. The magnitude of the resonance component is assessed as about 6 kcal mol⁻¹. This value increases by ca. 1 kcal mol⁻¹ on going from the weak to strong resonance-assisted hydrogen bonding. The magnitude of the hydrogen bonding component varies in the wide range from 2 to 20 kcal mol⁻¹ depending on the structure of the β-diketone in question.     

基于辐射声功率最小化的安静结构设计

本文研究了一种基于模型修改使结构辐射声功率最小的方法，使用了结构动力学、声学和优化理论等学科知识，对结构修改后固有频率变化可以忽略不计时的声辐射优化进行了研究，将设计变量看作外部阻抗，对结构的表面振速进行了重新分布，可以降低结构辐射的声功率。将质量块与动力吸振器进行组合实现声辐射最小化，不但降低了一定频率范围内的平均声功率，还降低了动力吸振器所对应的单频下的声功率；运用遗传算法搜索结构辐射声功率最小时附加质量块或动力吸振器的位置，对附加质量块和有源控制作用下简支钢板的声功率最小化进行了比较研究，阐明了附加外部结构与有源控制实现安静结构的物理机理。最后，对本文提出的基于平板辐射声功率最小化的安静结构设计方法进行了实验验证。     

粒径可控的纳米铁酸铋的制备及其光催化性能

采用改进的聚丙烯酰胺凝胶法制备了BiFeO3纳米颗粒,利用热重-差热、红外光谱及X射线衍射等手段研究了干凝胶的热分解及BiFeO3的成相过程.结果表明,在600℃煅烧可制备出高纯的BiFeO3纳米颗粒.同时发现,随着双丙烯酰胺含量的增加,所得样品晶粒尺寸逐渐减小,从而制备出平均粒径约52～110nm的系列BiFeO3颗...     

梯度下降法在沉积物粒度分布拟合中的应用

结合实测数据,以三个对数正态分布函数的和函数为拟合函数,以梯度下降法为主要方法,对沉积物粒度分布进行了数据拟合,通过数值实验我们发现:利用梯度下降法可以有效地优化分布函数的各参数,实现拟合残差的稳步持续减小,具有良好的可操作性,拟合效果是令人满意的,它为我们进行数据拟合提供了一条新的思路,同时此方法也可以推广到解决其他极值问题.     

Hydrogen bond donors and acceptors are generally depolarized in α-helices as revealed by a molecular tailoring approach

Hydrogen-bond (H-bond) interaction energies in α-helices of short alanine peptides were systematically examined by precise density functional theory calculations, followed by a molecular tailoring approach. The contribution of each H-bond interaction in α-helices was estimated in detail from the entire conformation energies, and the results were compared with those in the minimal H-bond models, in which only H-bond donors and acceptors exist with the capping methyl groups. The former interaction energies were always significantly weaker than the latter energies, when the same geometries of the H-bond donors and acceptors were applied. The chemical origin of this phenomenon was investigated by analyzing the differences among the electronic structures of the local peptide backbones of the α-helices and those of the minimal H-bond models. Consequently, we found that the reduced H-bond energy originated from the depolarizations of both the H-bond donor and acceptor groups, due to the repulsive interactions with the neighboring polar peptide groups in the α-helix backbone. The classical force fields provide similar H-bond energies to those in the minimal H-bond models, which ignore the current depolarization effect, and thus they overestimate the actual H-bond energies in α-helices. © 2019 The Authors. Journal of Computational Chemistry published by Wiley Periodicals, Inc.     

Tightly coupled aeroelastic model implementation dedicated to fast aeroelastic tailoring optimisation of high aspect ratio composite wing

This paper presents the development of a code, called GEBTAero, dedicated to very flexible aircraft (VFA) aeroelasticity and especially the evaluation of aeroelastic tailoring effect on critical speeds. GEBTAero is an open source code consisting in a tightly coupling between a geometrically exact beam theory -and a finite state induced flow unsteady aerodynamic model, including an homogenisation tool. This model has been implemented in Fortran using GEBT code and optimised open source libraries with particular focus on computation speed. Besides a non linear transient dynamic simulation capacity, a particular focus is put on the fast critical speed computation strategy using a non-iterative modal approach about the geometrically non linear deformed shape of the wing with the computation of only a few aeroelastic modes. Computation speed and accuracy of this implementation is assessed using widely used aeroelastic test cases and compared successfully to other aeroelastic codes. Configurations using aeroelastic tailoring, which are the core target of this solver, are then evaluated numerically on a representative high aspect ratio anisotropic composite wing and a simple 2-ply composite laminates with both variable ply orientations. It illustrates the strong correlation between the structural bending/twisting coupling of an unbalanced composite laminates and its critical aeroelastic speed. It also shows the high sensitivity of ply orientation on the aeroelastic behaviour.