共振条件下载波包络相位效应对阈上电离谱的影响

本文通过求解三维含时薛定谔方程, 从理论上研究了共振条件下氢原子的光电子能谱与角分布随着激光脉冲载波包络相位(CEP)的变化规律. 研究结果表明: 在共振位置附近, 光电子能谱的强度与CEP有强烈的依赖关系; 进一步对各个分波的分析, 可以确定共振电离初态的角量子数. 此外, 利用光电子的角分布信息, 可以对多周期激光脉冲的初始相位信息进行高精度探测. 关键词： 阈上电离 超短脉冲 载波包络相位     

Angular distributions for double ionization of Li- by an ultrashort, intense laser pulse.

We predict photoelectron angular distributions for double ionization of Li- by both weak and intense ultrashort, linearly polarized laser pulses by direct numerical integration of the three-dimensional, time-dependent Schr?dinger equation. Li- is treated as a two-active electron system. Near threshold, for low intensity we recover general features of angular distributions for one-photon double ionization. For the intense field (multiphoton) case, the photoelectron angular distribution changes significantly, particularly in directions parallel and perpendicular to the laser polarization axis.     

Photoelectron angular distributions in resonant multiphonon ionization of atoms

Conclusions It has been demonstrated that photoelectron angular distributions in resonant multiphoton ionization depend critically on the angular momentum quantum numbers of the intermediate state. This should help to interpret the spectra of atoms more complex than alkalies. In addition, information about the matrix elements for the bound-free transition can be obtained which is not available if the angle-integrated ionization cross section is measured. Reliable cross sections for photoionization out of excited atomic states are very important for astrophysics, but so far only a few laboratory data are available. The interpretation of some of these data is not straightforward, however, because of lack of knowledge about the degree of alignment of the atoms in the excited state. This problem can be solved either by optically pumping the atom into only one magnetic sublevel [24] or by measuring the photoelectron angular distribution in addition to the absolute cross section.Sektion Physik der Universitat München, D-8046 Garching, FRG. JILA Visiting Fellow, 1980–1981. Joint Institute for Laboratory Astrophysics, National Bureau of Standards and University of Colorado, Boulder, Colorado 80309. Published in Primenenie Lazerov v Atomnoi, Molekulyarnoi i Yadernoi Fiziki-Trudy II Vsesoyuznoi Shkoly, pp. 12–23, 1981.     

原子激发态在高频强激光作用下的光电离研究

本文通过数值求解动量空间的三维含时薛定谔方程, 研究了原子高激发态在高频激光脉冲作用下, 在电离阈值附近的光电子能谱和两维动量角分布. 研究结果表明: 在该能量范围内, 单光子电离过程的贡献是最主要的. 体系初态的主量子数可以由光电子能谱峰值的位置来确定; 体系初态的角量子数可以通过光电子的两维动量角度分布确定. 在比较宽泛的参数范围内, 这一规律不随入射激光的强度和脉冲时间宽度的改变而改变, 因此原则上可以利用它对原子的初态进行识别. 此外, 还研究了体系的初态为相干叠加态, 光电子动量谱随着叠加态相对相位的变化规律. 关键词： 阈上电离 激发态 高频激光脉冲 两维动量角度分布     

Competition of resonant and nonresonant paths in resonance-enhanced two-photon single ionization of He by an ultrashort extreme-ultraviolet pulse

We theoretically study the pulse-width dependence of the photoelectron angular distribution (PAD) from the resonance-enhanced two-photon single ionization of He by femtosecond (?20 fs) extreme-ultraviolet pulses, based on the time-dependent perturbation theory and simulations with the full time-dependent Schr?dinger equation. In particular, we focus on the competition between resonant and nonresonant ionization paths, which leads to the relative phase δ between the S and D wave packets distinct from the corresponding scattering phase shift difference. When the spectrally broadened pulse is resonant with an excited level, the competition varies with pulse width, and, therefore, δ and the PAD also change with it. On the other hand, when the Rydberg manifold is excited, δ and the PAD do not much vary with the pulse width, except for the very short-pulse regime.     

Strong field modifications of photoelectron angular distributions in resonant two-photon ionization

The two symmetry parameters β₂ and β₄, which govern completely the photoelectron angular distribution in resonant two-photon ionization, are found to depend strongly on the electric field strength of the light pulse.     

The effects of self-induced resonance in multiphoton ionization

The ionization of atoms in the presence of an intermediate two-photon resonance is considered. The ionization probability and spectral distribution of the ionized electrons are obtained for the case when the resonant is turned on adiabatically. The limiting cases of small and large ionization widths are investigated. At sufficiently large intensities of the resonant field an essential asymmetry in the ionization probability depending on the sign of the two-photon detuning is obtained.     

Ar原子序列双光双电离产生光电子角分布的理论计算

基于多组态Dirc-Fock方法和密度矩阵理论,给出了原子序列双光双电离光电子角分布的计算表达式,发展了相应的计算程序.利用该程序对Ar原子3p壳层序列双光双电离过程进行了理论研究,给出了光电离的总截面、磁截面、剩余离子取向以及光电子角分布的各向异性参数与入射光子能量的函数关系.结果显示在光电离截面的Cooper极小位置附近取向参数出现极大值,而光电子角分布的各向异性参数在该位置附近出现极小值.进一步给出了33.94和55.34 eV光子能量下序列双光双电离过程中第一步的Ar原子和第二步的Ar^+离子3p壳层光电子角分布,分析了序列双光双电离光电子角分布与单光电离光电子角分布的差异.将计算结果与文献已有的数据进行了比较,具有很好的一致性.本文的研究结果对揭示光与物质相互作用的非线性动力学机制具有重要的参考价值.     

利用强场多光子电离技术实现对多原子分子离子振动量子态的光学操控

利用飞秒光电子影像技术研究了碘甲烷分子在飞秒强激光场作用下的多光子电离动力学,在实验上实现了运用飞秒强场多光子电离技术对多原子分子离子的振动量子态进行光学操控.提高了飞秒激光的强度,从1.6×1013W/cm2提高到2.5×1013W/cm2.在增大的激光强度范围内,发现了新的能量组分,并对此进行归属.通过采集光电离的光电子影像可以得到强场电离后光电子的动能分布和角度分布两方面的信息,前期的研究主要侧重于讨论光电子动能随光强的变化,重点讨论了光电子角度分布随光强的变化,通过观察光电子角度分布的变化趋势对振动量子态调控机理进一步认识.     

Two-photon resonant three-photon ionization with ultrashort pulses

The problem of two-photon resonant three-photon ionization is analysed for the case of ultrashort ionizing pulses. An analytic solution to the problem is obtained and discussed. A simple experiment is proposed which would demonstrate the effect of optical nutation on the photoelectron flux.     

Two-step excitation of an auto-ionized state of the Ba atom associated with two-photon excitation of an intermediate state

An experimental and theoretical study is performed of the angular photoelectron distribution for three-photon ionization of Ba atoms through the 2ω-excited intermediate state 6p ²(¹ S ₀) and the auto-ionized state 6p8s(³ P ₁). Rotation of the polarization plane of dye-laser radiation allowed us to investigate the photoelectron angular distribution. Electrons were counted with the help of a time-of-flight electron spectrometer. The density-matrix formalism is used to obtain expressions for the angular dependence of the differential ionization probability. Possible experiments are discussed. Zh. éksp. Teor. Fiz. 113, 834–840 (March 1998)     

Observation of large quadrupolar effects in a slow photoelectron imaging experiment

We have studied nondipolar effects in resonance-enhanced multiphoton ionization of Xe and have observed an azimuthal dependence of the photoelectron angular distribution on a quadrupole resonance, as well as a very large asymmetry with respect to the direction of the laser propagation close to the resonance, which is understood in terms of interference between dipole- and quadrupole-allowed ionization channels. The observed asymmetry in the photoelectron angular distribution provides insight into the ejection of slow photoelectrons near an ionization threshold.     

Ionization of a multilevel atom by ultrashort laser pulses

Specific features of ionization of single atoms by laser fields of a near-atomic strength are investigated. Calculations are performed for silver atoms interacting with femtosecond laser pulses with wavelengths λ = 800 nm (Ti:Sapphire) and λ = 1.064 μm (Nd:YAG). The dependences of the probability of ionization and of the form of the photoelectron energy spectra on the field of laser pulses for various values of their duration are considered. It is shown that the behavior of the probability of ionization in the range of subatomic laser pulse fields is in good agreement with the Keldysh formula. However, when the field strength attains values close to the atomic field strength, the discrepancies in these dependences manifested in a decrease in the ionization rate (ionization stabilization effect) or in its increase (accelerated ionization) are observed. These discrepancies are associated with the dependence of the population dynamics of excited discrete energy levels of the atom on the laser pulse field amplitude.     

Angular distribution of the photoelectron spectra for ethylene,propylene, butene and butadiene

The photoelectron spectra using the He I resonance line (21.22 eV) were measured for ethylene, propylene, 1-butene, cis-butene, trans-butene and 1,3-butadiene as a function of angle between the direction of the incoming photons and outgoing photoelectrons. From these data the angular parameter, β, is obtained for each photoelectron peak in each spectrum. The β value is a function of the energy of the photoelectron and the nature of the molecular orbital from which the photoelectron is ejected. A qualitative comparison is made between the experimentally derived β values and the molecular orbital assignments. In particular, it is noted that the photoelectron peak corresponding to the CC double bond π orbital yields a relatively high value of β. This has led in the case of butadiene to a confirmation that the first two photoelectron peaks both result from ionization in π orbitals.     

Femtosecond coincidence imaging of multichannel multiphoton dynamics

The novel technique of femtosecond time-resolved photoelectron-photoion coincidence imaging is applied to unravel dissociative ionization processes in a polyatomic molecule. Femtosecond coincidence imaging of CF3I photodynamics illustrates how competing multiphoton dissociation pathways can be distinguished, which would be impossible using photoelectron or ion imaging alone. Ion-electron energy correlations and photoelectron angular distributions reveal competing processes for the channel producing (e(-)+CF+3+I). The molecular-frame photoelectron angular distributions of the two major pathways are strikingly different.     

Angular distribution of electrons during two-photon ionization of atoms by elliptically polarized radiation

Two-photon ionization of the hydrogen-like uranium ion by elliptically polarized radiation is investigated in the present work. It is demonstrated that the fundamental effect of interference of the probability amplitudes arises in the angular photoelectron distribution when the degree of ellipticity of ionizing radiation is varied. Translated from Izvestiya Vysshikh Uchebnykh Zavedenii, Fizika, No. 12, pp. 39–41, December, 2008.     

Excited hydrogenic atom in a strong low-frequency electromagnetic field

The multiphoton ionization of a bound electron state which is twofold degenerate with respect to its orbital angular momentum is considered in a quasiclassical approximation. It is shown that the ionization probability increases strongly in an intense electromagnetic field, in which nonresonant mixing of the levels forming the degenerate state is significant, in comparison to the case described by the Keldysh formula. It is also shown that such degeneracy leads to a sharp increase in the intensity of the radiation scattered by the bound electron, and the high-frequency cutoff of the emission spectrum is shifted to higher frequencies. Zh. Tekh. Fiz. 69, 15–20 (August 1999)     

Multiphoton atomic ionization in the field of a very short laser pulse

Closed analytic expressions are derived for the probability of multiphoton atomic and ionic ionization in a variable electric field ?(t), which are applicable for arbitrary Keldysh parameters γ. Dependencies of the ionization probability and photoelectron pulse spectrum on the shape of a very short laser pulse are analyzed. Examples of pulse fields of various forms, including a modulated light pulse with a Gaussian or Lorentz envelope, are considered in detail. The interference effect in the photoelectron energy spectrum during atomic ionization by a periodic field of a general form is examined. The range of applicability of the adiabatic approximation in the multiphoton ionization theory is discussed. The imaginary time method is used in the calculations, which allows the probability of particle tunneling through oscillating barriers to be effectively calculated.     

双共振激发多光子电离过程中电离光电子谱的量子相干调制

利用缀饰态和微扰理论,研究了双共振激发多光子电离过程中电离光电子谱的量子相干特性,讨论了强场作用下激发脉冲的面积和脉冲间的延迟对多光子电离光电子谱的影响.结果表明,脉冲面积和脉冲间的延迟对电离光电子谱有明显的调制作用.当第一个脉冲的面积和脉冲间的延迟选取合适时,实现了多光子电离光电子谱Autler-Townes分裂以及电离光电子谱中干涉条纹的控制,并且利用这一量子相干控制实现了粒子在两个缀饰态之间的选择性布居;第二个脉冲面积的变化不影响两个缀饰态上的粒子布居几率,但对电离光电子谱有着明显的调制作用.     

Angular distribution of the photoelectron spectrum of CO2, COS,CS2, N2O,H2O,and H2S

The photoelectron spectra of the triatomic molecules CO₂, COS, CS₂, N₂O, H₂O, and H₂S have been measured as a function of the angle θ between the direction of the incoming photon and outgoing photoelectron. The photoelectron spectra have been measured with a double-focusing electrostatic electron spectrometer to which has been attached a chamber containing a gas discharge lamp that can be freely rotated. (The photon source used was the 21.22 eV He I resonance line). From the dependence of intensity as a function of θ the angular parameter β was determined for each ionization band observed in the photoelectron spectra. A correlation was noted between the values of β and the molecular orbitals relative to the contributions of oxygen and sulfur atomic orbitals. Individual β values were also obtained for most of the vibrational bands seen in the photoelectron spectra. In most cases the vibrational structure showed little or no change in the angular parameter for a given electronic state. In certain cases, however, such as the fourth ionization band in CS₂, CO₂, and COS, rather sizeable changes in β were observed for the different vibrational bands.