Discrimination of Excited States of Acetylacetone through Theoretical Molecular-Frame Photoelectron Angular Distributions

Photoelectron angular distribution (PAD) in the laboratory frame for randomly oriented molecules is typically described by a single anisotropy parameter, the so-called asymmetry parameter. However, especially from a theoretical perspective, it is more natural to consider molecular photoionization by using a molecular frame. The molecular frame PADs (MFPADs) may be used to extract information about the electronic structure of the system studied. In the last decade, significant experimental efforts have been directed to MFPAD measurements. MFPADs are highly characterizing signatures of the final ionic states. In particular, they are very sensitive to the nature of the final state, which is embodied in the corresponding Dyson orbital. In our previous work on acetylacetone, a prototype system for studying intra-molecular hydrogen bond interactions, we followed the dynamics of the excited states involved in the photoexcitation–deexcitation process of this molecule. It remains to be explored the possibility of discriminating between different excited states through the MFPAD profiles. The calculation of MFPADs to differentiate excited states can pave the way to the possibility of a clear discrimination for all the cases where the recognition of excited states is otherwise intricate.     

FS and FS(OH) defect centers at the MgO(1 0 0) surface: cluster and periodic calculations

We present a model of a new paramagnetic defect center which results from the interaction of atomic hydrogen with the MgO(1 0 0) surface. DFT calculations have been performed using periodic supercells and embedded cluster models where long-range polarization effects are included explicitly. The H atom promotes the creation of an oxygen vacancy (F center) by formation of the F_S⁺(OH⁻) defect where an hydroxyl group is adsorbed near an electron trapped in an oxygen vacancy. This new center has some characteristics similar to those of the classical F_S⁺ centers but a smaller formation energy; furthermore, being globally neutral, it can be treated also with supercell methods.     

Cu(1 1 1) and Cu(0 0 1) surface electronic states. Comparison between theory and experiment

Recent advances in both the experimental resolution and in the computational capabilities motivate new studies of surface properties. In particular, a detailed comparison between theoretical and experimental data is expected to provide a better insight into surface and image states. In this work we present a joint effort analyzing such features of the Cu(1 1 1) and Cu(0 0 1) surfaces. The experiments are performed by using both linear and non-linear angle-resolved photoemission. From the theoretical point of view, we make use of the Green function embedding technique within density functional theory. We are able to account for the image states by suitably modifying the effective potential in the Kohn-Sham equation and the generalized boundary conditions on the Green function. Comprehensive theoretical and experimental results on the effective mass and the binding energy of the Shockley state and the first image states are reported.     

第一性原理研究Fe掺杂SnO2材料的光电性质

采用基于第一性原理的线性缀加平面波(FP-LAPW)方法,研究Fe掺杂SnO₂材料电子结构和光学性质,包括电子态密度、能带结构、介电函数和其他一些光学图谱. 研究结果表明,掺Fe后材料均属于直接跃迁半导体,且呈现半金属性;随掺杂浓度增加,费米能级进入价带,带隙逐渐减小,Fe原子之间耦合作用增强;通过掺杂能够在一定程度上改变成键性质,使其具有金属键性质. 光学谱线(吸收谱、消光系数等)与介电函数虚部谱线相对应,均发生蓝移,各峰值与电子跃迁吸收有关,从理论上指出光学性质和电子结构的内在联系. 关键词： 能带结构 态密度 光学性质 介电函数     

吸附氢分子的振动态及熵的计算

用第一性原理方法研究了H_2在(MgO)_9及(AlN)_(12)团簇上的吸附态、振动模式及熵.分析表明,吸附体系的振动中有六个简正模式可归为氢分子的振动;由于氢分子质量很小,零点能修正对吸附能有重要影响.利用振动配分函数计算了吸附氢分子的熵,表明吸附态H_2的熵主要决定于较低的同相振动的频率,并不完全与吸附强度相关;在标准大气压下70—350 K的温度范围内,吸附H_2的熵与气态H_2的熵之间存在很好的线性关系,吸附后H_2的熵减小约10.2R.     

柱状分层固体媒质的声散射

本文评述了各向同性和横向各向同性柱状分层固体声散射理论和实验研究进展 ,介绍了描述圆柱状界面薄层特性的弹簧模型 ,也讨论了该领域中有待进一步研究的一些问题。     

Atomic NOON state generation in distant cavities by virtual excitations

A general scheme of generating NOON states of virtually-excited 2N atoms is proposed. The two cavities are fibre-connected with N atoms in each cavity. Although we focus on the case of N = 2, the system can be extended to a few atoms with N 〉2. It is found that all 2N atoms can be entangled in the form of NOON states if the atoms in the first cavity are initially in the excited states and atoms in the second cavity are all in the ground states. The feasibility of the scheme is carefully discussed, it shows that the NOON state with a few atoms can be generated with good fidelity and the scheme is feasible in experiment.     

双势垒磁性隧道结中量子阱共振隧穿效应的第一性原理理论

磁性隧道结材料中自旋相关的量子阱态所导致的共振隧穿现象具有很重要的研究和应用价值，文章介绍了最近在Fe（001）／MgO／Fe／MgO／Fe双势垒磁性隧道结中存在的量子阱共振隧穿效应的理论研究工作，通过量子阱态的第一性原理的计算以及结合对中间Fe薄膜孤岛结构所导致Coulomb阻塞效应的分析，证实了最近Nozaki等人（Nozaki T et al．Phys．Rev．Lett．，2006，96：027208）实验中得到的振荡效应确实来源于中间Fe层多数自旋电子在Г点处形成的△1对称性的量子阱态．Coulomb阻塞效应的存在正是导致实验中低温下量子阱共振隧穿效应不够明显的主要原因．     

Anti-diffusion method for interface steepening in two-phase incompressible flow

In this paper, we present a method for obtaining sharp interfaces in two-phase incompressible flows by an anti-diffusion correction, that is applicable in a straight-forward fashion for the improvement of two-phase flow solution schemes typically employed in practical applications. The underlying discretization is based on the volume-of-fluid (VOF) interface-capturing method on unstructured meshes. The key idea is to steepen the interface, independently of the underlying volume-fraction transport equation, by solving a diffusion equation with reverse time, i.e. an anti-diffusion equation, after each advection time step of the volume fraction. As the solution of the anti-diffusion equation requires regularization, a limiter based on the directional derivative is developed for calculating the gradient of the volume fraction. This limiter ensures the boundedness of the volume fraction. In order to control the amount of anti-diffusion introduced by the correction algorithm we propose a suitable stopping criterion for interface steepening. The formulation of the limiter and the algorithm for solving the anti-diffusion equation are applicable to 3-dimensional unstructured meshes. Validation computations are performed for passive advection of an interface, for 2-dimensional and 3-dimensional rising-bubbles, and for a rising drop in a periodically constricted channel. The results demonstrate that sharp interfaces can be recovered reliably. They show that the accuracy is similar to or even better than that of level-set methods using comparable discretizations for the flow and the level-set evolution. Also, we observe a good agreement with experimental results for the rising drop where proper interface evolution requires accurate mass conservation.