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122.
Chunhong Wang Qi Cui Zhixin Zhang Prof. Zhu-Jun Yao Dr. Shaozhong Wang Prof. Zhi-Xiang Yu 《Chemistry (Weinheim an der Bergstrasse, Germany)》2019,25(42):9821-9826
1,3-Azaprotio transfer of propargylic α-ketocarboxylate oximes, a new type of alkynyl oximes featuring an ester tether, has been explored by taking advantage of gold catalysis. The incorporation of an oxygen atom to the chain of alkynyl oximes led to the formation of two different oxa-cyclic nitrones. It was found that internal alkynyl oximes with an E-configuration deliver five-membered nitrones, whereas terminal alkynyl oximes with an E-configuration afford six-membered nitrones. DFT calculations on four possible pathways supported a stepwise formation of C−N and C−H bonds, in which a 1,3-acyloxy-migration competes with the 1,3-azaprotio-transfer, especially in the case of internal alkynyl oximes. The relative nucleophilic properties of oxygen in the carbonyl group and the nitrogen in the oxime, the electronic effects of alkynes, and the influence of the ring system have been investigated computationally. 相似文献
123.
Shi-Chun Mao Zhaohui Zhang Jiansen Gao Zhen-Sen Wu 《Waves in Random and Complex Media》2019,29(1):54-62
A solution to the problem of Gaussian beam scattering by an anisotropically coated circular cylinder is presented. The incident Gaussian beam source is expanded as an approximate expression in the simple form with a Tayor’s series. The transmitted field in the anisotropically coated region is expressed as a infinite summation of eigen plane waves with different polar angles. The unknown coefficients of the scattered fields are obtained with the aid of the boundary conditions. The infinite series can be truncated under the prerequisite of achieving the solution convergence. Only the case of transverse-electric polarization is discussed. The similar formulation of transverse-magnetic polarization can be obtained by adopting the similar method. Some numerical results are presented and discussed. The result is in agreement with that available as expected when the Gaussian beam degenerates to a plane wave incidence case. 相似文献
124.
Nonlinear Dynamics - Global dynamics of a flexible asymmetrical rotor resting on vibrating supports is investigated. Hamilton’s principle is used to derive the partial differential governing... 相似文献
125.
Prof. Jen-Shyang Ni Tianliang Min Yaxi Li Menglei Zha Dr. Pengfei Zhang Prof. Chun Loong Ho Prof. Kai Li 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(25):10265-10271
Planar luminogens have encountered difficulties in overcoming intrinsic aggregation-caused emission quenching by intermolecular π-π stacking interactions. Although excited-state double-bond reorganization (ESDBR) can guide us on designing planar aggregation-induced emission (AIE) luminogens (AIEgens), its mechanism has yet been elucidated. Major challenges in the field include methods to efficiently restrict ESDBR and enhance AIE performance without using bulky substituents (e.g., tetraphenylethylene and triphenylamine). In this study, we rationally developed fluoro-substituent AIEgens with stronger intermolecular H-bonding interaction for restricted molecular motions and increased crystal density, leading to decreased nonradiative decay rate by one order of magnitude. The adjusted ESDBR properties also show a corresponding response to variation in viscosity. Furthermore, their aggregation-induced reactive oxygen species (ROS) generations have been discovered. The application of such planar AIEgen in treating multidrug-resistant bacteria has been demonstrated in a mouse model. The relationship between ROS generation and distinct E/Z-configurational stacking behaviors have been further understood, providing a design principle for synthesizing planar AIEgen-based photosensitizers. 相似文献
126.
排名聚合将多个排名列表聚合成一个综合排名列表,可应用于推荐系统、链路预测、元搜索、提案评选等.当前已有工作从不同角度对不同排名聚合算法进行了综述、比较,但存在算法种类较少、数据统计特性不清晰、评价指标不够合理等局限性.不同排名聚合算法在提出时均声称优于已有算法,但是用于比较的方法不同,测试的数据不同,应用的场景不同,因此何种算法最能适应某一任务在很多情况下仍不甚清楚.本文基于Mallows模型,提出一套生成统计特性可控的不同类型的排名列表的算法,使用一个可应用于不同类型排名列表的通用评价指标,介绍9种排名聚合算法以及它们在聚合少量长列表时的表现.结果发现启发式方法虽然简单,但是在排名列表相似度较高、列表相对简单的情况下,能够接近甚至超过一些优化类方法的结果;列表中平局数量的增长会降低聚合排名的一致性并增加波动;列表数量的增加对聚合效果的影响呈现非单调性.整体而言,基于距离优化的分支定界方法 (FAST)优于其他各类算法,在不同类型的排名列表中表现非常稳定,能够很好地完成少量长列表的排名聚合. 相似文献
127.
Understanding and control of the surface properties such as molecular orientations are of great importance in numerous applications of ionic liquids. However, there remain discrepancies among the previous experimental and theoretical studies on the surface orientation and structures of room temperature ionic liquids(RTIL) systems. In this article, the orientation of 1-butyl-3-methylimidazolium([bmin]) cation at the air/liquid interface of a characteristic RTIL, 1-butyl-3-methylimidazolium hexafluorophosphate([bmim][PF6]), was investigated by the sum frequency generation vibrational spectroscopy(SFG-VS). Detailed polarization and experimental configuration analyses of the SFG-VS spectra showed the possibility of a small spectral splitting in the CH3 symmetric stretching region, which can be further attributed to the probable existence of multiple orientations for the interfacial [bmim] cations. In addition, the(N)–CH3 vibrations were absent, ruling out the prediction by several recent molecular dynamics simulations which state that portions of the [bmim] cations orient with a standing-up(N)–CH3 group at the ionic liquid surface. Hence, new realistic theoretical models have to be developed to reflect the complex nature of the ionic liquid surface. 相似文献
128.
129.
金属光阴极因其超短脉冲发射和运行寿命长的特性从而具有重要应用价值,但是较高的功函数和较强的电子散射使其需要采用高能量紫外光子激发且光电发射量子效率极低.本文利用Mie散射共振效应增强银纳米颗粒中的局域光学态密度,提升光吸收率和电子的输运效率,并利用激活层降低银的功函数,从而增强光阴极在可见光区的量子效率.采用时域有限差分方法分析银纳米球阵列的光学共振特性,采用磁控溅射和退火工艺在银/氧化锡铟复合衬底上制备银纳米球,紧接着在其表面沉积制备铯激活层,最后在高真空腔体中测试光电发射量子效率.实验结果表明平均粒径150 nm的银纳米球光阴极在425 nm波长的量子效率超过0.35%,为相同激活条件下银薄膜光阴极的12倍,峰值波长与理论计算的Mie共振波长相符合. 相似文献
130.
Jinke Bai Linfeng Wang Wenyong Chen Xiao Jin Qinghua Li Yuxiao Wang Xueru Zhang Yinglin Song 《Particle & Particle Systems Characterization》2020,37(8):2000115
Device grade quantum dots (QDs) require QDs ensembles to retain their original superior optical properties as in solution. QDs with thick shells are proven effective in suppressing the inter-dot interaction and preserving the emission properties for QDs solids. However, lattice strain–induced defects may form as the shell grows thicker, resulting in a notable photoluminescence quenching. Herein, a well-type CdxZn1−xS/CdSe/CdyZn1−yS QDs is proposed, where ternary alloys CdZnS are adopted to match the lattice parameter of intermediate CdSe by separately adjusting the x and y parameters. The resultant thick-shell Cd0.5Zn0.5S/CdSe/Cd0.73Zn0.27S QDs reveal nonblinking properties with a high PL QY of 99% in solution and 87% in film. The optimized quantum dot light-emitting diodes (QLEDs) exhibit a luminance of 31547.5 cd m−2 at the external quantum efficiency maximum of 21.2% under a bias of 4.0 V. The shell thickness shows great impact on the degradation of the devices. The T50 lifetime of the QLEDs with 11.2 nm QDs reaches 251 493 h, which is much higher than that of 6.5 and 8.4 nm QDs counterparts. The performances of the well-type thick-shell QLEDs are comparable to state-of-the-art devices, suggesting that this type of QDs is a promising candidate for efficient optoelectronic devices. 相似文献