Strengthened Hyper-Raman Lines with the Coherent Superposition State

High-order harmonic generations from a one-dimensional Coulomb potential atom are calculated with the initial state prepared as a coherent superposition between its ground and first excited states. When the energy difference of the two states is small, we can choose proper laser pulse such that the first excited state can be excited only to other bound states instead of being ionized. We show that only the hyper-Raman lines are observable instead of the harmonics. The energy difference of the ground and the first excited state can be deduced from the highest peak of the hyper-Raman lines. We further show that the similar results can be obtained by using a combination of two laser pulses with different frequencies interacting with the atom initially at the ground state.     

Giant resonances on excited states

We derive modified RPA equations for small vibrations about excited states. The temperature dependence of collective excitations is examined. The formalism is applied to the ground state and the first excited state of ⁹⁰Zr in order to confirm a hypothesis which states that not only the ground state but every excited state of a nucleus has a giant resonance built upon it.     

The single-determinant approximation with a local potential for excited states

The specific features of the calculations of the electronic structure in the approximation of a local exchange potential that is identical for all the electrons involved are considered. An optimized effective potential method is proposed for calculating the energies of excited electronic states of the same symmetry. A single-particle Schrö dinger equation is derived for an excited state whose orbitals are described by a single-determinant wave function orthogonal to the ground state. The equations determining the local potential for excited states are obtained within the variational approach. The solution to these equations is analyzed in the framework of the parameterized representation of the effective potential. The efficiency of the proposed method is demonstrated by calculating the energies of three excited states of the same symmetry for a HeH molecule. The difference between the results obtained by the Hartree-Fock method and the method proposed in this paper is equal, on average, to 0.05%. A comparison with the results obtained from precise calculations based on the configuration interaction method shows that the accuracy in determining the energy of the excited states by the optimized effective potential method is comparable to the accuracy in calculating the energy of the ground state.     

基态和单态第一激发态的联氨单分子分解反应的密度泛函研究

本文运用密度泛函B3LYP/6-311+G(3df,2p)方法研究了联氨分子的电子结构和能量,并系统分析了联氨分子的分解反应,计算绘制了单分子联氨在基态和单态第一激发态下沿N-N分解反应的势能曲线。本文计算发现联氨分子在这两种电子态下的离解能分别是：基态58.8 kcal/mol,单态第一激发态495.5 kcal/mol。基态分子分解反应是吸热反应,而单态第一激发态分解反应是放热反应。计算发现单态第一激发态的激发能是554.2 kcal/mol。结合这两种电子态下联氨分子的红外振动频率分析,本文认为,在非强制断键的情况下,联氨分子沿N-N键均裂而生成两个NH2自由基的可能性很小。     

叠加激发双模压缩真空态的量子统计特性(英文)

从激发双模压缩真空态a^+mb^+m|ξ>出发构造了叠加态|Ψ>,研究了|Ψ>的量子统计特性.结果表明:在一定的条件下,随着相位差的变化,叠加态|Ψ>的平均光子数出现类似于Rabi振荡的崩塌与复原现象,而且与单个激发双模压缩真空态a^+mb^+m|ξ>相比,在叠加态|Ψ>中光场的相位压缩和亚泊松光子统计特性都得到了加强.     

基态和单态第一激发态的联氨单分子分解反应的密度泛函研究

本文运用密度泛函B3LYP/6-311+G(3df,2p)方法研究了联氨分子的电子结构和能量,并系统分析了联氨分子的分解反应,计算绘制了单分子联氨在基态和单态第一激发态下沿N-N分解反应的势能曲线。本文计算发现联氨分子在这两种电子态下的离解能分别是：基态58.8 kcal/mol,单态第一激发态495.5 kcal/mol。基态分子分解反应是吸热反应,而单态第一激发态分解反应是放热反应。计算发现单态第一激发态的激发能是554.2 kcal/mol。结合这两种电子态下联氨分子的红外振动频率分析,本文认为,在非强制断键的情况下,联氨分子沿N-N键均裂而生成两个NH2自由基的可能性很小。     

High-order harmonic generation spectrum of an excited one-dimensional Coulomb atom in an intense laser field

Response of the wave packet of a one-dimensional Coulomb atom to an intense laser field is calculated using the symmetrized split operator fast Fourier method. The high-order harmonic generation (HHG) of the initial state separately being the ground and excited states is presented. When the hardness parameter \alpha in the soft Coulomb potential V(x)=-1/\sqrt{x^2+\alpha} is chosen to be small enough, the so-called hard Coulomb potential V(x)=-1/|x| can be obtained. It is well known that the hard one-dimensional Coulomb atom has an unstable ground state with an energy eigenvalue of $\sim0.5$ and it has no states corresponding to physical states in the true atoms, and has the first and second excited states being degenerate. The parity effects on the HHG can be seen from the first and second excited states of the hard one-dimensional Coulomb atom. The HHG spectra of the excited states from both the soft and hard Coulomb atom models are shown to have more complex structures and to be much stronger than the corresponding HHG spectrum of the ground state of the soft Coulomb model with $\alpha=2$ in the same laser field. Laser-induced non-resonant one-photon emission is also observed.     

Role of excited states in the elliptically polarized harmonic generation

We theoretically investigate the contribution of the excited state to the ellipticity of the harmonics from H＋ at different orientation angles irradiated by a linearly polarized laser pulse. It is found that the first excited state has a significant influence to the ellipticity of the harmonics, and the contribution of higher excited states to the ellipticity can be neglected. Moreover, the conclusion is not dependent on the laser intensity.     

Spectral line suppression and sideband narrowing via quantum interference

We reveal that for a realistic system, interference effects are obtained such as the suppression of central line and inner sidebands and the narrowing of the outer fluorescence sidebands. For this purpose, we consider a spontaneous decay from an excited state to a metastable state when the excited and metastable states are resonantly coupled to an auxiliary metastable state by a laser field and a microwave field, respectively. The fluorescence spectrum evolves from a five-peaked structure into a doublet of ultrasharp lines as the ratio of the laser field Rabi frequency to the microwave Rabi frequency is decreased. The physical origin is presented in terms of dressed states.     

Ultrahigh Harmonic Generation from an Atom with Superposition of Ground State and Highly Excited States

We investigate the high-order harmonic generation from an atom prepared in a superposition of ground state and highly excited state. When the atom is irradiated by an ultrashort pulse, the cutoff position of the plateau in the harmonic spectrum is largely extended compared with the case that the atom is initially in the ground state. The physics of the extension of the high-order harmonic plateau can be interpreted by the spatial structure of the atomic initial wave packet. We can optimize the generation of high-order harmonics by substituting the excited state for a particular coherent superposition of some highly excited states to form a spatially localized excited wave packet.     

Correspondence of Fluorescing States of Naphthols and Naphtholate Anions and its Effect on the Calculation of pKa∗ from Spectral Shifts

The validity of dissociation constants of electronically excited acids and bases, calculated from spectral shifts^1,2 accompanying protolytic dissociation, especially where shifts of fluorescence spectra are employed, is dependent, among other factors, upon fluorescence orginating from excited states of the same electronic configuration in both acid and conjugate base.³ In some of the molecules whose excited state acid-base properties have been most extensively studied, notably some derivatives of naphthalene, energy level reversals have been shown to accompany dissociation in the lowest excited singlet state in aqueous solutions.⁴ The spectroscopic properties and excited state dissociation phenomena of the naphthols have been studied extensively from several points of view.^5-9 While the calculation of the excited state dissociation properties of β-naphthol, in which fluorescence occurs from the ¹L_b state in both anion and neutral molecule, presents no particular problem with regard to correspondence of the lowest excited singlet states of conjugate acid and base, it appeared that in α-naphthol, by analogy with α-naphthylamine⁴, fluoescence might occur from the ¹L_a state in the conjugate base and from the ¹L_b state in the conjugate acid. Thus it seemed that a careful consideration of the states from which the fluorescences of the conjugate species derived from α-naphthol in fluid aqueous solutions orginated, would be useful.     

弯曲振动引致的过渡态的混沌

从单摆运动的特征出发 ,指出分子的过渡态 (包括解离时的态 ) ,如分子内弯曲振动引致结构变化的过渡态 ,必然伴随着混沌现象 ,而且和Chirikov的多重共振会导致混沌的观点有关 .并以从HCN、HNC和其非局域态的高激发振动态的能级拟合得到的弯曲模式的性质说明这个观点 .最后 ,提出一个处理弯曲振动引致的过渡态的混沌的物理模型 .     

Photon-number distribution of two-mode squeezed thermal states by entangled state representation

Using the entangled state representation, we convert a two-mode squeezed number state to a Hermite polynomial excited squeezed vacuum state. We first analytically derive the photon number distribution of the two-mode squeezed thermal states. It is found that it is a Jacobi polynomial; a remarkable result. This result can be directly applied to obtaining the photon number distribution of non-Gaussian states generated by subtracting from (adding to) two-mode squeezed thermal states.     

Resonance-Raman-induced Kerr effect in molecules in the ground and electronically excited states

A theoretical investigation of the resonantly enhanced, Raman-induced Kerr effect (resonance-RIKE) is given, taking into account the resonance absorption of the laser wave and the population of excited electronic states. Line shape, maximum amplification and optimum conditions for the resonance-RIKE from the ground state as well as for the resonance-RIKE from an initial excited electronic state are discussed in detail. The possibility is studied of applying this method to the investigation of the vibrational structure of excited electronic states in molecules.     

壳模型对13N Gamow-Teller跃迁的研究

最近的研究表明¹³N的beta衰变对于Ia型超新星爆炸前的电子丰度有着重要的影响.本文在壳模型的基础上,首先计算¹³N基态到基态以及基态到不同激发态的Gamow-Teller(GT)跃迁强度,并将其与实验数据进行了比较.在理论计算的GT强度基础上,对不同温度和密度天体环境下¹³N的电子俘获率进行了细致的计算,并重点讨论基态到激发态的GT跃迁对电子俘获率变化的影响.结果表明,考虑基态到激发态的跃迁后,超新星的电子丰度下降,中微子能量损失增大.基态到激发态跃迁对电子俘获率的影响主要由低激发能级贡献. 关键词： Gamow-Teller跃迁 壳模型 电子俘获 激发态     

Energy and Electron Transfer in the Field of Transition Metal Complexes

The bimolecular quenching of an excited state molecule in fluid solution can occur in three fundamental ways:^1–3 (i) chemical reaction between the excited state and the quencher, (ii) electronic energy transfer from the excited state to the quencher, or (iii) deactivation of the excited state by some catalytic action of the quencher. The intimate nature of the quenching mechanism is often difficult to elucidate for a single excited state-quencher couple. More useful information can generally be obtained from correlations of data concerning homogeneous families of excited states and/or quenchers.     

Rb原子激发态碰撞能量转移

报道了用连续单模激光激发Rb原子至特定的激发态，从而观察激发态间的碰撞形成更高Rb原子激发态的实验结果.实验观察到Rb原子激发态的自发辐射与高激发态的碰撞形成通道之间的明显竞争，测得了高激发态的形成概率与激发光功率、原子蒸气温度及激光失谐的关系，所提出的碰撞能量转移机理较好地解释了实验结果. 关键词：     

Holographic insulator/superconductor phase transitions with excited states

We construct a family of solutions of the holographic insulator/superconductor phase transitions with the excited states in the AdS soliton background by using both the numerical and analytical methods. The interesting point is that the improved SturmLiouville method can not only analytically investigate the properties of the phase transition with the excited states, but also the distributions of the condensed fields in the vicinity of the critical point. We observe that, regardless of the type of the holographic model, the excited state has a higher critical chemical potential than the corresponding ground state, and the difference of the dimensionless critical chemical potential between the consecutive states is around 2.4, which is different from the finding of the metal/superconductor phase transition in the Ad S black hole background. Furthermore, near the critical point, we find that the phase transition of the systems is of the second order and a linear relationship exists between the charge density and chemical potential for all the excited states in both s-wave and p-wave insulator/superconductor models.     

量子限制效应对δ掺杂GaAs/AlAs多量子阱中铍受主态寿命的影响

采用远红外时间分辨光谱,研究了量子限制效应对δ掺杂在GaAs/AlAs多量子阱中铍（Be）受主态寿命的影响.在低温下的远红外吸收谱中,清楚地观察到了三条主要吸收线,它们分别来源于铍受主从基态到它的三个奇宇称激发态的跃迁.实验结果表明：随着量子限制效应的增强,受主激发态寿命而减少,实验测得体材料中Be受主2p激发态的寿命是350 ps,而阱宽10 nm的多量子阱中的寿命是55 ps.量子限制效应对布里渊区折叠声学声子模的影响增强了受主带内空穴与声学声子相互作用,从而加快了受主带内空穴的弛豫过程. 关键词： 量子限制效应 受主态寿命 时间分辨光谱 δ掺杂')" href="#">δ掺杂     

H_2~+分子与共振相关的阈下谐波的取向效应

通过数值模拟的方法研究了H_2~+阈下谐波的取向效应.数值模拟过程中,主要关注波长为760nm的阈下谐波,通过逐次减去激发态贡献的方法,研究共振相关谐波不同取向角下的变化规律.结果表明:阈下平行、垂直谐波展示的复杂取向依赖与共振效应密切相关,该现象主要由与基态共振的各激发态的轴对称性导致.另外,用包含跃迁偶极子的简单模型对取向效应进行了概括描述,并以H_2~+第一激发态为演化初始态进行了验证.本文结果可为阈下谐波取向效应的实验研究提供参考.