利用极化拍频光谱术研究光子回波

利用相位共轭极化拍频光谱术对Ｖ型三能级系统中的光子回波进行了研究,当抽运光束为宽带线宽且相对时间延迟〉０时,单光子四波混频对应于三脉冲受激光子回波。抽运光束为宽带线宽且相对时间延心〈０的情形与抽运光束为窄带线宽的情形类似,这种技术在测量激发态之间的能级分裂时,可得到消除多谱勒增宽的测量精度。     

反-4,4''-双(N,N-二丁胺基)二苯乙烯分子双光子吸收性质研究

对于实验室合成的反-4,4'-双(N,N-二丁胺基)二苯乙烯分子,实验测量了该分子的单光子和双光子荧光谱,然后从理论上研究了其单光子和双光子吸收特性.研究结果表明,在低能量范围内,分子的单光子吸收主要发生在分子的第一激发态,而分子的双光子吸收主要发生在分子的第二和第四激发态上.该分子在相应系列衍生物中具有最大的双光子吸收截面.分子的相关能对分子的激发态能量影响较大.我们给出了分子基态与电荷转移态的电荷转移过程,并从理论上定性解释了双光子聚合反应的聚合机理.     

Semiclassical theory of the radiative-collisional cascade in a Rydberg atom

We have developed a two-dimensional semiclassical model of the radiative-collisional cascade for hydrogen-like systems. We describe the collisions with electrons and ions by classical diffusion in the space of principal and orbital quantum numbers and use an iterative procedure that consistently takes into account the quantum nature of the radiative cascade for radiative transitions. The model establishes the correspondence between the quantum and classical approaches and indicates that the latter cannot be directly used to calculate the population kinetics of highly excited atomic states. Our calculations of the two-dimensional populations of highly excited atomic hydrogen states for selective, three-body, and photorecombination sources of population allow the data of one-dimensional kinetic models to be refined. The calculated intensities of recombination lines demonstrate the degree of nonequilibrium of the Rydberg state populations under typical astrophysical plasma conditions.     

Multiphoton ionization and dissociation of CH3I at 266 and 355 nm

The mechanisms of multiphoton ionization (MPI) and dissociation of CH3I have been studied using timeof-flight (TOF) mass spectrometer at 266 and 355 nm. MPI mass spectrum at 266 nm consists mostly of fragment ions. This is consistent with a neutral-fragment photoionization mechanism in which rapid one-photon dissociation occurs from the repulsive potential energy surface followed by MPI of neutral photofragments. The observation of parent ions at 355-nm excitation is indicative of parent-ionic ladder mechanism in which the parent ions are produced directly by two-photon excitation resonantly excited to Rydberg C state and then ionized through additional one-photon absorption to produce CH3I+. Fragment ions are produced by dissociation of CH3I+.     

AlK壳层等离子体辐射谱模型的比对

碰撞辐射模型的比对研究对校验发展等离子体辐射谱模型、提高等离子体参数的诊断精度具有重要意义. 基于Al等离子体, 对常用的辐射模型代码FAC和FLYCHK K壳层辐射谱模型开展了比对研究, 详细比较了它们的离子丰度、特征线强度、谱发射率曲线和吸收系数曲线等特征, 并根据各能态的速率方程, 从FAC和FLYCHK模型的结构特点出发, 分析了造成这些差异的原因. FAC 和FLYCHK计算得到的类H、类He离子n=2, n=3激发态数密度有显著差异, 进而引起特征线发射率及其比值(He-IC/He-αup, He-βup/H-βup)的差异, 从而对等离子体参数的诊断结果产生影响. 除了模型中采用的能级结构和碰撞辐射过程速率外, 计算结果显著地受到FAC 和FLYCHK 模型结构的影响. n=2激发态数密度的差异是由FAC和FLYCHK分别采用能级和超组态(组态)的方式构建n=2激发态的速率方程而引起的, 而FAC代码忽略了n=3与更高激发态之间的碰撞耦合过程, 是引起n=3激发态数密度差异的原因. 主要特征线的吸收系数与基态能级的数密度相关, 受到激发态数密度的影响较小, 因此与谱发射率曲线相比, FAC和FLYCHK计算结果的差异更小.     

Strong coupling in macrocyclic thiophene investigated by time-resolved two-photon excited fluorescence

We report the femtosecond dynamics of fluorescence anisotropy excited through the two-photon absorption (TPA), which provides direct signatures of delocalized electronic excitations for symmetrical macromolecular architectures. Two-photon excited fluorescence anisotropy is strongly correlated with the orientation and value of the transition moment from the excited state to the second and higher lying states. For macromolecular systems it leads to a relatively low initial fluorescence anisotropy and specific femtosecond anisotropy dynamics. We have experimentally demonstrated qualitatively different anisotropy dynamics for two- and one-photon absorption excitations for strongly coupled ring architecture prospective for artificial-light-harvesting applications and possessing an enhanced TPA-absorption cross section.     

二苯乙烯衍生物分子双光子吸收截面：官能团对称性的影响

选取了具有不同对称性的二苯乙烯系列衍生物分子，在HF水平上，利用响应函数方法，研究了该系列分子的单光子和双光子特性. 研究结果表明，该系列分子具有较强的双光子特性. 在可见光范围内，反对称分子的最大双光子吸收态是第一激发态，而对称分子的最大双光子吸收出现在第四激发态. 相对于对称分子而言，反对称分子具有更大的双光子吸收截面. 因此，分子的对称性是否比不对称性更有利于增大分子的双光子吸收截面，还与分子的π中心部分的特性有关. 还给出了电荷转移态的电荷迁移过程. 关键词： 双光子吸收 响应函数方法 非线性光学     

Multiphoton Spectra and States of Halogens

Abstract

Although the diatomic halogens are endowed with a wide range of intravalence-shell electronic states, the number and variety of these states is far from obvious in one-photon absorption from the ground state where only a few regions of structured absorption are present at visible and UV wavelengths. Selection rules on angular momentum and parity are key players in enforcing this sparse structure, but Franck- Condon effects also exercise considerable influence by directing transitions into regions where the transition dipole is small o r into a continuum where much of the detail is lost: further, a simultaneous excitation of two o r more electrons is formally forbidden in single-photon transitions. Some of the obstacles to one-photon absorption are avoided in the sequential absorption of two o r three photons using the conveniently placed, low-lying excited sQtes in the visible region for the initial step, in effect broadening the perspective from the ground state to include that from the lower excited states. This article summarizes progress realized by classical and nonclassical (multiphoton) methods of spectroscopy which, over the last 10–12 years, has led to the identification of many new states of halogens and materially improved the definition of several known ones. The advances are timely in that the same period has witnessed a renewal of interest in halogen spectra, largely because of their use in rare-gas halide lasers but also because the homonuclear halogens and certain interhalogens have potential value as laser systems in their own right [1, 2].     

The Influence of Particles Interaction in Low-Temperature Plasma on its Composition and Optical Properties

A model theory of the influence of particles interaction in plasma on its composition and optical properties is developed. The interaction of charged particles in plasma reduces the ionization energy of atoms and ions. The action of internal microfields in plasma on atoms and ions reduces the statistical weight of electron levels which affects the populations of excited states. The latter effect leads to an effective cutoff of partition functions and determines the behaviour of optical properties of plasma (of absorption coefficient and emissivity) at increased number densities of charged particles. The formulas are obtained for calculation of the continuous and discrete spectrum in plasma taking into account the particles interaction. A non-monotonic dependence of optical plasma density upon number density of charged particles is quantitatively explained. A satisfactory agreement is obtained with a large number of experimental data some of which were considered to be contradictory. The method developed can be used for calculations in the field of atomic spectroscopy and low-temperature plasma physics including increased densities of charged particles. The use of the formulas obtained in plasma diagnostics will enable one to avoid considerable errors.     

General theory of radiative corrections to atomic decay rates

A general expression is derived for the radiative corrections to the one-photon decay rates of hydrogen-like ions. Our approach is based on the evaluation of the imaginary part of the fourth-order Lamb shift for excited states. We thereby avoid the ambiguities connected with electron wave function renormalization. The result may be cast in a form which is manifestly gauge invariant. As an application, we show that the formulas used by Lin and Feinberg in their study of relativistic M1 transitions, obtained by heuristic arguments, are derivable from first principles.     

Microscopic theory of optical excitations,photoluminescence, and terahertz response in semiconductors

This article presents a comprehensive many-body theory for optically excited semiconductors. The coupled equations of motion for the correlation functions of the Coulomb-interacting electron-hole system are derived and solved for different excitation conditions. The generation of a coherent excitonic polarization and its conversion into incoherent populations is analyzed. The spontaneous emission properties of the excited system are evaluated using a fully quantized theory. Luminescence from excitonic and electron-hole plasma populations is computed, and significant hole burning in the exciton center of mass distributions is predicted. It is shown how different excitations states of the many-body system can be identified by their characteristic signatures in the absorption spectra of a terahertz probe field.     

Determination of radiative lifetimes of neutral sulphur by time-resolved three-photon VUV laser spectroscopy

Radiative lifetimes of the highly exited states s and d of neutral sulphur have been measured using time-resolved laser-induced fluorescence. The sulphur atoms were generated in a laser-produced plasma. The investigated states were populated through a two-step process involving a two-photon excitation to the lowest excited triplet state of even parity , followed by a one-photon excitation to the investigated state. We obtained ns and ns. These values are much longer than theoretically predicted ones and much shorter than those indirectely inferred from astronomical data. Received: 9 February 1998 / Accepted: 24 February 1998     

Two-photon photoionization by singlet–singlet annihilation in polycrystalline,thin perylene films

Two-photon photoionization processes in thin, polycrystalline, α- and β-crystalline perylene films have been investigated for photon energies at the optical absorption threshold. The kinetic energy of the emitted electrons is found to be essentially independent of the photon energy, indicating that geometrically relaxed excited states are involved. The high ionization yield at such low photon energies is therefore attributed rather to the annihilation of adiabatically relaxed singlet excitons than to the direct two-photon ionization process. This leads to hole final states different from those obtained in one-photon, vertical ionization processes.     

Optical Bloch equations with dual photon excitation explain the polarization dependence of four wave mixing quantum beats

We explain the polarization dependence of four wave mixing (FWM) quantum beats for semiconductors as essentially due to the spin phase correlations of photo-excited electrons, rather than to Coulomb interaction between the electrons. A theoretical analysis is given within the framework of optical Bloch equations for the light–semiconductor interactions and the Luttinger–Kohn model for the band structure. Residual Coulomb interactions between charge carriers are ignored. The results suggest that the polarization dependence of FWM quantum beats is a purely coherent effect of dual photon excitations, rather than, e.g., exciton–exciton Coulomb interaction. We show that the coherence transfer between the excited states is responsible for the FWM in a configuration with orthogonally polarized pump and probe.     

Dynamical structure factor of a one-dimensional harmonic liquid: Comparison of different approximation methods

The optical properties of Anderson-localized many-particle excitations in doped crystals are discussed assuming that the direct interaction between the active ions is greater than their interaction with the radiation field. It is shown that in this case the Anderson localization of the excitation energy on a finite number of ions has no influence in zeroth order on the absorption and emission properties at low excitation intensities used in conventional spectroscopy. Only at higher excitation intensities resulting in multiply excited many-ion states are characteristic quenching effects of the luminescence expected. These become evident by a conversion of the multiply excited states into fast relaxing, degenerate states either of the ions themselves or of the host lattice. These quenching effects offer possibilities to determine experimentally the number of coherently coupled ions forming the many-particle Anderson-localized excitations.     

Cluster states prepared by using hot trapped ions

We propose a scheme for the preparation of one-dimensional and two-dimensional cluster states by using hot trapped ions. The scheme is based on the interaction between two ions and bichromatic radiation. The vibrational mode in our protocol is only virtually excited so that the system is insensitive to the thermal field. In addition, we only use two levels of ions as qubits and the successful probability may achieve 100%.     

Theory of pressure-induced vibrational and rotational absorption of diatomic molecules colliding with atoms at high temperatures

A derivation is given for the integrated absorption coefficient of pressure-induced pure rotational and vibrational transitions in binary collisions of homonuclear diatomic molecules with neutral atoms. The previously neglected effects of excited vibrational states, mechanical anharmonicity, vibration-rotation interaction, transverse components of the dipole moment, and a higher order term in the expansion of the z component of the dipole moment are taken into account to obtain more accurate absorption coefficients at temperatures above 423 K. In the region of the fundamental wave number the excited vibrational states make more of a contribution to the absorption than their relative populations would indicate.     

以芘为中心系列衍生物的单光子和双光子吸收特性理论研究

在含时密度泛函理论的水平上,利用响应场理论方法研究了以芘为中心系列衍生物的单光子和双光子吸收特性. 研究结果表明,在低能量范围内,每个分子有多个电荷转移态. 单光子吸收性质与实验结果符合较好. 随着分子尺寸的增加,分子的最大双光子吸收截面显著增加,其中具有四分枝结构分子的最大双光子吸收截面是单枝结构分子的5.6倍. 同时,分子的双光子吸收截面与分子结构的对称性有关.其中对称结构分子具有较大的双光子吸收截面.     

Luminescence of CdS generated by high intensity excitation below the bandgap

High excitation photoluminescence of CdS at low temperatures excited by photons below the bandgap show the same general features as those obtained by one-photon band to band absorption. The excitation spectrum of the M-line shows no structure corresponding to a giant two-photon absorption expected for the direct creation of excitonic molecules.     

The features of nonlinear absorption during resonance one- and two-photon excitation of the basic exciton transition in colloidal CdSe/ZnS quantum dots

The features of the nonlinear absorption of CdSe/ZnS quantum dots (colloidal solution) in the case of resonant one- and two-photon excitation of the basic exciton transition by powerful ultra-short laser pulses were determined. In one-photon excitation, with an increasing intensity of impulses, a decrease in absorption (bleaching) is relayed by an increase in absorption, which is associated with the process of the filling of the states (saturation) of a two-level system with the lifetime of the excited state depending on the light intensity. The arising Fresnel or Fraunhofer diffraction of the laser ray that pass through a colloidal solution with a high concentration of quantum dots is associated with the formation of the transparency channel and self-diffraction of laser ray on an induced diaphragm. In two-photon excitation, the features of the nonlinear absorption and luminescence tracks (the dependence of luminescence intensity on distance) were explained by the influence, in addition to the two-photon absorption, of the processes that are responsible for the slower growth of nonlinear absorption and luminescence quenching at high intensities of laser pulses.