Ultrafast photoionization of ions and molecules by orthogonally polarized intense laser pulses: Effects of the time delay

We present the photoelectron momentum distributions(PMDs) and the photoelectron angular distributions(PADs) of He+ ions, aligned H2+ molecules and N2 molecules by intense orthogonally polarized laser pulses. Simulations are performed by numerically solving the corresponding two-dimensional time-dependent Schr?dinger equations(TDSEs) within the single-electron approximation frame. Photoelectron momentum distributions and photoelectron angular distributions present different patterns with the time delays Td, illustrating the dependences of the PMDs and PADs on the time delays by orthogonally polarized laser pulses. The evolution of the electron wavepackets can be employed to describe the intensity of the PADs from the TDSE simulations for N2 molecules.     

线偏振双色激光场中氪原子的阈上电离现象

采用基于Guo,Aberg和Crasemann发展的强激光场中的非微扰量子散射理论(GAC理论),研究了线偏振双色激光场中氪(Kr)原子阈上电离的光电子角分布,双色激光场由一系列相同的单周期激光脉冲组成.研究发现光电子角分布有强烈的位相依赖关系,且呈现出反演不对称性、喷射结构和展宽结构等现象,这为实验上通过改变双色激光场的相对相位来观察和控制光电子角分布提供了一种有效的方法.     

Angular distributions of fast electrons, ions, and Bremsstrahlung x/gamma-rays in intense laser interaction with solid targets

We study the angular distributions of fast electrons, ions, and bremsstrahlung x/ gamma-rays generated during the interaction of an ultrashort intense laser pulse with solid targets. A relation is found on the angular directions for fast electrons and ions as a function of the particle's kinetic energy, experienced Coulomb potential changes, and the incident angle of the laser pulse. It is valid independent of the acceleration mechanisms and the polarization of the laser pulse, as confirmed by particle-in-cell simulations. The angular distribution of bremsstrahlung x/gamma-rays is presented to show explicitly its correlation with the corresponding angular distributions of electrons.     

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.     

Multiphoton electron angular distributions from laser-aligned CS2 molecules

Laser-aligned carbondisulfide (CS2) molecules are singly ionized by multiphoton absorption from intense, linearly polarized 25 fs laser pulses. The angular distribution of the photoelectrons exhibits a significant dependence on the angle between the polarizations of the aligning and ionizing laser fields. The widely used strong-field approximation predicts angular distributions in qualitative agreement with the experimental data but fails at a quantitative level.     

Ionic Angular Distributions Induced by Strong-Field Ionization of Tri-Atomic Molecules

Angular distributions of fragment ions from ionization of several tri-atomic molecules(CO_2, OCS, N_2O and NO_2) by strong 800-nm laser fields are investigated via a time-of-flight mass spectrometer. Anisotropic angular distributions of fragment ions, especially those of atomic ions, are observed for all of the molecules studied.These anisotropic angular distributions are mainly due to the geometric alignment of molecules in the strong field ionization. Distinct different patterns in ionic angular distributions for different molecules are observed. It is indicated that both molecular geometric structure and ionization channels have effects on the angular distributions of strong field ionization/fragmentation.     

Mev X rays and photoneutrons from femtosecond laser-produced plasmas

We demonstrate a novel method to monitor the total angular distribution of the spectrum of hard x-ray emission from a plasma generated with femtosecond laser pulses with an intensity of 5 x 10(18) W/cm2 on a solid target. Measured and calculated angular distributions of x rays show a pronounced anisotropy for MeV photon energies. We complemented the spectral information by demonstrating a (gamma,n) nuclear reaction with a tabletop laser system.     

Role of highest occupied molecular orbitals in molecular field-free alignment by a femtosecond pulse

This paper studies the molecular rotational excitation and field-free spatial alignment in a nonresonant intense laser field numerically and analytically by using the time-dependent Schr?dinger equation. The broad rotational wave packets excited by the femtosecond pulse are defined in conjugate angle space, and their coefficients are obtained by solving a set of coupled linear equations. Both single molecule orientation angles and an ensemble of O₂ and CO molecule angular distributions are calculated in detail. The numerical results show that, for single molecule highest occupied molecular orbital (HOMO) symmetry σ tends to have a molecular orientation along the laser polarization direction and the permanent dipole moment diminishes the mean of the orientation angles; for an ensemble of molecules, angular distributions provide more complex and additional information at times where there are no revivals in the single molecule plot. In particular, at the revival peak instant, with the increase of temperature of the molecular ensemble, the anisotropic angular distributions with respect to the laser polarization direction of the π _g orbital gradually transform to the symmetrical distributions regarding the laser polarization vector and for two HOMO configurations angular distributions of all directions are confined within a smaller angle when the temperature of the molecular ensemble is higher.     

How to measure the internuclear vector from photoelectron angular distributions

This paper uses a nonperturbative scattering theory to study photoelectron angular distributions of homonuclear diatomic molecules irradiated by circularly polarized laser fields. This study shows that the nonisotropic feature of photoelectron angular distributions is not due to the polarization of the laser field but the internuclear vector of the molecules. It suggests a method to measure the molecular orientation and the internuclear distance of molecules through the measurement of photoelectron angular distributions.     

Photoelectron spectra from multiple ionization of atoms in ultra-intense laser pulses

We address the question of the energy and angular distributions of the photoelectrons ejected from rare gas atoms submitted to ultra-intense infrared laser pulses, with peak intensities I(max) approximately 10(18) W/cm (2). Several unsolved issues regarding the angular distributions of the photoelectrons are analyzed. We believe that our results should help to trigger new investigations.     

Rescattering of electrons at laser-cluster interactions

The goal of this work is to derive the angular distributions of electrons irradiated at the outer ionization of large atomic clusters from Xe atoms by relativistic laser pulses taking into account rescattering processes. Both the magnetic field of the laser pulse and the Coulomb field of the ionized cluster significantly influence the rescattering of ejected electrons. The multiply inner ionization of atoms occurs at the leading edge of the laser pulse. The atomic ions with charge multiplicities up to Z = 26 are subsequently produced (each atomic ion with the next charge multiplicity appears in 3–5 fs) when the laser intensity increases. The measurements of the angular distributions of electrons allow us to reproduce the imaging dynamics of outer ionization of the cluster at the leading edge of the relativistic femtosecond laser pulse.     

Microobject manipulations using laser beams with nonzero orbital angular momentum

Microobject manipulation with a laser is investigated. The functional capabilities of the laser manipulators can be significantly enhanced using beams with predetermined distributions of intensity and angular momentum. Beams with nonzero angular momentum are generated using phase and amplitude-phase masks. Such beams make it possible to rotate weakly absorbing particles and to move them along a given trajectory. Experimental results on the microobject motion along various trajectories (circle, triangle contour, self-intersecting curve, and Archimedes spiral) are presented.     

Velocity map imaging study of OCS photodissociation followed by S(1S) autoionization at 157 nm

Atomic sulphur ions (S+) were observed directly by crossing a carbonyl sulphide (OCS) molecular beam with a F2 laser. In this study both S+ ion and electron images were measured using the velocity map imaging technique. The results imply that S+ is produced from the well-known photodissociation of OCS at 157 nm leading to the dominant S(1S) + CO(1Σ+) channel, and then the excited S(1S) atom is directly ionized by another 157 nm photon. Correlated vibrationally resolved angular distributions and internal energy distribution of the CO coproducts are reported here and compared with previous studies. This experiment yields strong and sharp S+ images which may be useful for calibrating any imaging or laser ionization apparatus when using a 157 nm laser. A number of technical aspects such as corrections for partial slicing and imperfect laser polarization are described. Abstraction of product angular distributions using both polarized and unpolarized photolysis lasers is also demonstrated using velocity map imaging.     

Photoelectron angular distributions from two-photon ionization of atoms near ionization threshold

Photoelectron angular distributions(PADs) from two-photon ionization of atoms in linearly polarized strong laser fields are obtained in accordance with the nonperturbative quantum scattering theory.We also study the influence of laser wavelength on PADs.For two-photon ionization very close to the ionization threshold,most of the ionized electrons are vertically ejected to the laser polarization.PADs from twophoton ionization of atoms are determined by the second order generalized phased Bessel function at which the ponderomotive parameter plays a key role.In terms of dependence of PADs on laser wavelength,corresponding variations for the ponderomotive parameter are demonstrated.     

Molecular photoelectron momentum and angular distributions of N_2 molecules by ultrashort attosecond laser pulses

The ultrafast photoionization dynamics of N_2 molecules by x-ray/XUV laser pulses is investigated.The molecular frame photoelectron momentum distributions(MF-PMDs) and the molecular frame photoelectron angular distributions(MF-PADs) are obtained by numerically solving 2 D time-dependent Schrodinger equations within the single-electron approximation(SEA) frame.The results show that the molecular photoionization diffraction appears in 5 nm laser fields.However,when the laser wavelength is 30 nm,the molecular photoionization diffraction disappears and the MF-PMDs show four-lobe pattern.The ultrafast photoionization model can be employed to describe the MF-PMDs and MF-PADs of N_2 molecules.     

Eu原子4f~76p_(3/2)ns自电离衰变分支比和弹射电子角分布

首先运用孤立实激发技术将Eu原子从基态4f~76s~(28)S_(7/2)经中间态4f~76s6p共振激发到4f~76sns Rydberg态,然后再将其进一步激发至4f~76p_(3/2)ns(n=7,8)自电离态.其次,采用速度影像技术对Eu原子自电离弹射出的电子进行探测,以便来研究自电离衰变分支比和弹射电子角分布.在研究自电离衰变分支比时,重点讨论了粒子数反转的可能性,并依据此现象可为实现自电离激光器提供有价值的信息.另外,还探讨了各向异性参数对弹射电子角分布的影响;以及在Eu原子不同自电离几率位置处,讨论了弹射电子角分布形状的变化情况.     

Angular-resolved photoelectron spectroscopy of superatom orbitals of fullerenes

Photoelectron angular distributions from both C(60) and C(70) were recorded for low laser intensity femtosecond and picosecond pulses. Rich structure is seen for electron kinetic energies that lie below the photon energy. Strong, broad peaks are observed for photoelectron energies corresponding to single-photon ionization of so-called superatom molecular orbitals (SAMOs). The very simple angular distributions measured for these peaks, the close similarity of the spectra observed from C(60) and C(70), and the comparison with time-dependent density functional theory provide strong support for the SAMO hypothesis.     

Interference effects in the theory of multiphoton laser-simulated bremsstrahlung for electron wave packets that are broad in their momentum representation

The interference peculiarities of absorption and emission of external laser field quanta by a spatially narrow electron wave packet during its scattering at a potential center are considered. The angular and energy distributions for an electron due to scattering in a laser field are obtained and analyzed within the framework of the perturbation theory based on interaction with the potential center. A new mechanism of effective heating of plasma produced in a cluster under the effect of intense external laser field is found. Drastic changes in angular distribution due to the interference of incident and scattered parts of an electron wave packet are revealed.     

Threshold effects on angular distributions for multiphoton detachment by intense elliptically polarized light

Unusual threshold effects are found theoretically in the frequency and intensity dependence of angular distributions produced by an elliptically polarized laser as well as in the elliptic dichroism parameter, which measures the asymmetry of the angular distribution.     

Dynamic and geometric alignment of molecules induced by intense laser fields

We present a method to discuss simultaneously the relative importance of molecular dynamic and geometric alignment induced by intense laser fields in theoretical view. This method divides the process of molecular alignment into three steps, which are tightly correlated with that of molecular multielectron dissociative ionization and Coulomb explosion. A fourth-order Runge-Kutta algorithm and a developed counting approach are used to calculate the angular distribution of molecules in the first and second steps of molecular alignment. The last step is described by a field-ionization, Coulomb explosion model. The angular distribution of molecules at the critical distance originated from geometric alignment is obtained by calculating the volume of shells associated with a series of particular angle. The final angular distributions of molecules are obtained by properly weighting the results of three steps. The numerical results of distinguishing between dynamic and geometric alignment for certain conditions are presented and discussed. Our computational results show that the alignment mechanism, which dominates the observed anisotropy of angular distributions of ionic fragments for a given condition, is determined by the dependences of the extent of dynamic and geometric alignment on laser parameters and molecular parameters.