强场中NO分子回归谱的长程散射矩阵的理论研究

采用半经典散射矩阵方法研究外磁场中高里德伯态双原子分子在能量范围为77010—77050cm^-1的回归谱.通过引进模型势简化强磁场中NO分子的高里德伯电子的势函数,找出其在核转动量子数分别为N=1,3,5的三个通道中的闭合轨道,重点分析了强磁场中NO分子的长程散射矩阵元实部的傅里叶变换谱与闭合轨道之间的一一对应关系.     

平行电磁场中He+2的回归谱与闭合轨道的研究

利用半经典闭合轨道理论和分区自洽迭代方法计算了Rydberg态下He⁺₂在平行电磁场中的回归谱与闭合轨道. 为了模拟分子实的散射作用,引入一个包含电子交换势的新势能. 利用这一新势能,结合多通道量子亏损和分子闭合轨道理论,讨论了分子实散射效应对平行电磁场中He⁺₂的回归谱与闭合轨道的影响. 关键词： 回归谱 分子半经典闭合轨道 交换势 实散射     

强磁场中Rydberg NO分子的回归谱研究

利用分子的闭合轨道理论和多通道量子亏损理论,考虑核的转动影响,计算了Rydberg NO分子在外磁场中的回归谱.研究表明,复杂谱的结构可以用包含分子实散射的闭合轨道理论来解释,不管是同一通道内的弹性散射还是不同通道间的非弹性散射都起着非常重要的作用,尤其是较大标度作用量下,散射作用远大于基本轨道和重复轨道的贡献,很大程度上影响着体系的动力学性质。     

苯甲醇分子HOMO和N-HOMO轨道的电子动量谱学研究

利用第三代电子动量谱仪研究了苯甲醇(C_6H_5CH_2OH)分子的最高占据轨道(HOMO)和次最高占据轨道(N-HOMO)电子动量谱,给出了外价轨道的电离能谱信息.实验在非共面对称几何条件下完成,入射电子的能量为2400 eV加结合能.通过密度泛函方法计算得到了苯甲醇分子最高和次最高占据轨道的动量谱,理论与实验结果符合较好.     

垂直电磁场中He原子的吸收谱和回归谱的理论计算

半经典闭合轨道理论已经成功地计算了在外加磁场和平行电磁场中的里德堡原子的回归谱.但对于垂直电磁场中的里德堡原子,理论和计算都变得更为复杂.本文把闭合轨道理论推广到三维情况,采用 B.Hüpper的模型势计算了ε=-0.03,主量子数n≈ 40,m=0下He原子在垂直电磁场中的光吸收谱和回归谱,并和H原子在垂直电磁场中的回归谱作比较,突出了实散射的贡献.计算中应用了离子实散射的分区自洽迭代方法,并考虑到轨道的多次重复和离子实的多次散射效应.这是对闭合轨道理论的验证和进一步推广.     

TiO2表面氧空位对NO分子吸附的作用

采用程序升温热脱附(TPD)实验方法测定了NO在TiO2表面吸附后的脱附谱，利用分子轨道理论研究了TiO2吸附NO的原子簇模型及吸附前后的原子簇能级变化．结果表明，NO在TiO2表面吸附后可在两个峰值温度450和980K脱附出N2．TiO2表面经预覆氧处理后，N2的脱附量降低．吸附时NO中的O能够占据TiO2表面氧空位并与N脱离，而N原子则相互结合成为N2脱附．分子轨道理论计算证明在TiO2(110)表面能够存在氧空位并具备吸附NO的结构条件．     

探测二茂铁外价轨道(e,2e)反应中的扭曲波效应

利用第三代高效率电子动量谱仪,分别在600和1500 eV两种不同入射电子能量下获得了二茂铁(ferrocene)分子外价轨道的电离能谱和电子动量谱的相关实验结果.并利用非相对论与标量相对论密度泛函方法计算出了二茂铁的重叠型和交错型两种不同构象的理论动量谱.两种构象的外价轨道一一对应,理论电子动量谱基本一样.对二茂铁的外价轨道,在低动量区观测到了强烈的扭曲波效应,这与这些轨道主要由铁原子的3d轨道构成有关.通过相对论和非相对论计算结果的比较,表明相对论效应对于二茂铁的外轨道动量分布几乎没有影响. 关键词： 二茂铁分子 电子动量谱 相对论效应 扭曲波效应     

量子数亏损理论 多重散射计算方法

将多重散射自洽场方法和多通道量子数亏损理论结合,计算出分子的相互作用自洽势,对分子丰富的高激发态以及相应的连续态——分子的电离通道进行计算和分析,并给出了H_2,NO等分子的计算例子。     

并五苯分子光谱和激发态的密度泛函理论研究

采用密度泛函理论对并五苯分子做理论研究.在几何结构优化的基础上,对其进行频率分析得到了分子的红外光谱和喇曼光谱,并对谱线中的各峰值做了具体指认,同时也得到了分子的最高占据轨道和最低空轨道能隙为2.17 eV.利用含时密度泛函理论对其激发态计算,得到最低十个跃迁允许的单激发态.对前线分子轨道最高占据轨道和最低空轨道分析得到,C-C原子之间形成离域π键.结果表明：并五苯是一种良好的有机半导体材料,并具有很好的发光性能.     

环己烯分子2b和3a轨道的电子动量谱学研究

报道了环己烯(C6H10)分子2b和3a轨道电子动量谱的首次研究,并且给出了价轨道的电离能谱信息,实验在非共面对称几何条件下的能量多道型电子动量谱仪下完成,入射电子的能量为1200eV加结合能.通过Hartree-Fock和密度泛函方法计算得到了C6H10分子2b和3a轨道的动量谱,在动量大于0.25a.u.区域理论与实验结果符合较好,实验结果与理论计算相比在低动量端出现“上翘”的现象,这可能是由于分子的扭曲波效应引起的.     

Semiclassical calculation of Rydberg He2^＋ molecular of recurrence spectra ion in a magnetic field

Making use of the molecular closed-orbit theory and a new model potential for the Rydberg molecule, we have calculated the recurrence spectra of He^2＋ molecular ion in a magnetic field for different quantum defects. The Fourier transform spectra of He^2＋ molecular ion may be used to perform a direct comparison between peaks in the spectra and the scaled action values of closed orbits of the excited electron in external fields. We find that the spectral modulations can be analysed in terms of the scattering of the excited electron on the molecular core. Unlike the case of the Rydberg atom where the elastic scattering is predominant, modulations produced by inelastic scattering are also vital to the photoabsorption spectrum of the Rydberg molecule. Our results are in good agreement with the quantum results, which suggests that our method is correct.     

Absorption and Recurrence Spectra of Li Rydberg Atom in Perpendicular Electric and Magnetic Fields

We develop the semi-closed orbit theory from two degrees of freedom to three non-separable degrees of freedom and put forward a new model potential for the Li Rydberg atom, which reduces the study of the system to an effective one-particle problem. Using this model potential and the closed orbit theory for three degrees of freedom, we calculate the recurrence spectra of Li Rydberg atom in perpendicular electric and magnetic fields. The closed orbits in the corresponding classical system have also been obtained. The Fourier transformed spectra of Li atom have allowed direct comparison between the resonance peaks and the scaled action values of closed orbits, whereas the nonhydrogenic resonance can be explained in terms of the new orbits created by the core scattering. Our result is in good agreement with the quantum spectra, which suggests that our calculation is correct.     

Absorption and Recurrence Spectra of Li Rydberg Atom in Perpendicular Electric and Magnetic Fields

We develop the semi-closed orbit theory from two degrees of freedom to three non-separable degrees of freedom and put forward a new model potential for the Li Rydberg atom, which reduces the study of the system to an effective one-particle problem. Using this model potential and the closed orbit theory for three degrees of freedom, we caiculate the recurrence spectra of Li Rydberg atom in perpendicular electric and magnetic fields. The closed orbits in the corresponding classicai system have also been obtained. The Fourier transformed spectra of Li atom have ailowed direct comparison between the resonance peaks and the scaied action values of closed orbits, whereas the nonhydrogenic resonance can be explained in terms of the new orbits created by the core scattering. Our result is in good agreement with the quantum spectra, which suggests that our calculation is correct.     

Recurrence Spectra of the Rydberg Hydrogen Atom near Two Parallel Metal Surfaces

Using closed orbit theory, we study the influence of the two parallel metal surfaces on the recurrence spectra of a hydrogen atom placed in the region between the two surfaces. The results show that the metal surfaces have significant effect on the photoabsorption process. Each resonance peak in the recurrence spectra is associated with one electronic closed orbit. In our work, we put the first metal surface at the critical value dc and vary the second metal surface. The results show that when the distances between the hydrogen atom and the two metal surfaces are close to the critical valuedc, the number of the closed orbits is the greatest and there are more peaks in the recurrence spectra. When the distance between the atom and the second metal surface is larger or smaller than dc, the number of the closed orbits decreases and there are fewer peaks in the recurrence spectra. The agreement between the semiclassical calculation spectra and the quantum calculation spectra suggests that our analysis is correct.     

Broadening and shifts of molecular spectral lines by predissociation

The theory of predissociation is discussed for the broadening and shifts of molecular spectral lines. The application of the theory to the analysis of ultraviolet bands is based on the comparison between different isotopes of the same molecule. The theory is applied to absorption spectra of NO and good agreement is obtained with the experimental results.     

Recurrence spectra of He atoms in strong external fields

1 Introduction The photo-absorption phenomenon of high Rydberg atoms in strong external fields has attracted much attention in recent years. The semiclassical closed-orbit theory[1,2] developed by Du and Delos has been extensively used to explain this phenomenon. This theory has successfully calculated and interpreted the photo-absorption spectra of H- in various external fields[3,4] and has been applied to describe the photo-excitation, wave packet dynamics of some atoms and molecules such…     

Rydberg molecules in external fields: a semiclassical analysis

We analyze the spectra of simple Rydberg molecules in static fields within the framework of closed/periodic-orbit theories. We conclude that in addition to the usual classical orbits one must consider classically forbidden diffractive paths. Further, the molecule brings in a new type of "inelastic" diffractive trajectory in addition to the usual "elastic" diffractive orbits encountered in systems with point scatterers. The relative importance of inelastic versus elastic diffraction is quantified by merging the usual closed orbit theory framework with molecular quantum defect theory.     

First-principle study of NO adsorption on the LaFeO3 (0 1 0) surface

The adsorption of NO molecule on the LaFeO₃ (0 1 0) surface was studied using first-principle calculations based on density functional theory. The calculated results indicate that the Fe-top site is the most favorable for NO adsorption. The N-O bond length, Mulliken charge, and the N-O vibration frequency of the NO molecule are discussed after adsorption. The analysis results of the density of the states show that when NO is adsorbed with the Fe-NO configuration, the bonding mechanism is mainly from the interaction between the NO and the Fe d orbit.