芴二聚体三重激发态能量转移的理论研究

利用电子结构计算和电子转移速率理论,研究了芴二聚体的三重激发态能量转移过程. 应用限制性密度泛函理论构造得到非绝热态后,计算了控制能量转移的两个重要参数{电子耦合强度和重组能. 电子耦合强度的波动利用电子动力学模拟计算. 通过对上述参数相关函数的计算,成功得到了体系哈密顿量的对角元和非对角元波动,并应用微扰理论和波包扩散方法得到了能量转移速率. 结果表明,静态和动态的波动都明显地增加了能量转移速率,但是动态波动导致的速度增加却小于静态波动.     

Progress in improving thermodynamics and kinetics of new hydrogen storage materials

Hydrogen storage material has been much developed recently because of its potential for proton exchange membrane (PEM) fuel cell applications. A successful solid-state reversible storage material should meet the requirements of high storage capacity, suitable thermodynamic properties, and fast adsorption and desorption kinetics. Complex hydrides, including boron hydride and alanate, ammonia borane, metal organic frameworks (MOFs), covalent organic frameworks (COFs) and zeolitic imidazolate frameworks (ZIFs), are remarkable hydrogen storage materials because of their advantages of high energy density and safety. This feature article focuses mainly on the thermodynamics and kinetics of these hydrogen storage materials in the past few years.     

Quasi-classical Trajectory Study of Reaction O （^3P）＋HCl （v =2; j=1,6,9） →OH＋Cl

The reaction O（^3P）＋HCl （v=2; j= 1,6,9） → OH＋Cl is theoretically studied with a quasi-classical trajectory method （QCT） on the benchmark potential energy surface of the ground 3A＇＇ state [J. Chem. Phys. 119（2003）9550]. The QCT-calculated state-resolved rotational distributions are in good agreement with the experimental results. The rotational polarization of the product OH molecule becomes weaker as the initial HCl rotation is excited. The calculated results can be explained from the large mass factor cos2 β of the title reaction, the van der Waals well in the potential energy surface and the secondary encounters in the exit channel.     

High-Quality Large-Sized Single Crystals of Pb-Doped Bi2Sr2CuO6＋δ High-To Superconductors Grown with Traveling Solvent Floating Zone Method

High quality Pb-doped Bi2Sr2Cu06＋δ （Pb-Bi2201） single crystals are grown by the traveling solvent floating zone technique, with dimensions as large as - 50 min× - 5.0 min ×- 2 mm. The Pb-Bi2201 single crystals with different doping levels are obtained by the annealing process which covers a wide doping range of the overdoped region. We describe in detail the growth and annealing procedures and the characterization and physical property measurements of the Pb-Bi2201 crystals. The availability of these crystals provides a good opportunity to experimentally investigate high-To cuprate superconductors, particularly in the overdoped region.     

分子动力学模拟和自由能计算研究孕酮和孕酮受体蛋白的结合模式

孕酮在确立和维持妊娠中起到了关键的作用. 为了研究孕酮和孕酮受体蛋白的结合模式,进行了3.5纳秒的分子动力学模拟,用 MM-PBSA\GBSA方法计算了结合自由能. 自由能分解和丙氨酸扫描两种方法说明,残基 Leu718, Met756, Met759, Phe778 和 Tyr890 对于结合抑制剂作用明显,这些残基的主要作用能是范德瓦尔斯作用能. 这一研究结果可以指导孕酮受体蛋白抑制剂的优化     

碳纳米锥电子场发射的第一性原理研究

运用第一性原理研究了不同锥角和结构的碳纳米锥 （CNC） 电子场发射性能.结果表明：随外电场 （E_add） 增强,CNC电子结构变化显著,费米能级 （E_f） 处态密度 （DOS） 明显增大;赝能隙减小;体系电荷移向尖端.DOS,HOMO/LUMO及Mulliken电荷分析表明：CNC的电子场发射性能除依赖于尖端结构外,很大程度上还取决于锥角大小,特别顶层6个原子的CNC₃和CNC₄场发射性能 关键词： 碳纳米锥 电子场发射 第一性原理     

2-氨基吡啶气相氟代反应的密度泛函理论研究

采用量子化学方法,运用密度泛函理论(DFT)B3LYP方法,在6-311G*基组水平上,以2-氨基吡啶为起始反应物,全优化计算了亚硝酰阳离子NO~+对2-氨基吡啶中氨基进攻的重氮化反应及氟硼酸根阴离子BF_4~-对吡啶重氮正离子进攻的席曼反应的机理,搜索到整个反应过程中的过渡态结构,得到了反应路径并通过IRC验证,并对各反应中间体、过渡态和产物进行分子几何构型优化、振动频率分析和标准热力学函数计算.通过计算,搜索到的过渡态均为环状结构,与配位插入反应类似,利于原子间化学键的断裂及新键的形成;通过热力学及动力学计算,重氮化-席曼反应是剧烈的放热反应,与实验结果相吻合.     

Anisotropic Spin Splitting in Step Quantum Wells

By the method of finite difference, the anisotropic spin splitting of the AlxGa1-xAs/GaAs/Aly Ga1-yAs/AlxGal-xAs step quantum wells （QWs） are theoretically investigated considering the interplay of the bulk inversion asymmetry and structure inversion asymmetry induced by step quantum well structure and external electric field. We demonstrate that the anisotropy of the total spin splitting can be controlled by the shape of the QWs and the external electric field. The interface related Rashba effect plays an important effect on the anisotropic spin splitting by influencing the magnitude of the spin splitting and the direction of electron spin. The Rashba spin splitting presents in the step quantum wells due to the interface related Rashba effect even without external electric field or magnetic field.     

表面活性剂添加对水平管内气液两相流含液率的影响

应用电导断层测量技术研究表面活性剂添加对水平管内气液两相流含液率的影响,实验工质为空气/水、空气/100 mg/kg十二烷基硫酸钠(SDS)水溶液。结果表明,空气/水气液两相流动在光滑分层流型区,表面活性剂添加对平均截面含液率基本没有影响。随着液体流速的增加,空气/水气液两相流动进入波状分层流型区域,添加表面活性剂可以抑制或消除界面波动,增大平均截面含液率。表面活性剂的添加使弹状流含液率下降,气液流速较低时这一现象尤为明显。