Efficient solver for time-dependent Schrodinger equation with interaction between atoms and strong laser field

We present a parallel numerical method of simulating the interaction of atoms with a strong laser field by solving the time-depending Schr?dinger equation(TDSE) in spherical coordinates. This method is realized by combining constructing block diagonal matrices through using the real space product formula(RSPF) with splitting out diagonal sub-matrices for short iterative Lanczos(SIL) propagator. The numerical implementation of the solver guarantees efficient parallel computing for the simulation of real physical problems such as high harmonic generation(HHG) in these interaction systems.

Analysis of Potential Energy Surface for Butanone Isomerization

The potential energy surfaces for butanone isomerization have been investigated by density function theory calculation. Six main reaction pathways are confirmed using the intrinsic reaction coordinate method, and the corresponding isomerization products are 1-buten-2-ol, 2-buten-2-ol, butanal or 1-buten-l-ol, methyl 1-propenyl ether, methyl allyl ether, and ethyl vinyl ether, respectively. Among them, there are three pathways through butylene oxide, indicating butylene oxide is an important intermediate product during butanone isomer ization. The calculated vertical ionization energies of the reactant and its products are in a good agreement with the experimental values available. From the consideration for the relative energies Of transition states and the number of high-energy barriers we infer that the reaction pathway butanone-＊l-buten-2-ol---2-buten-2-oi is the most competitive. The obtained results are informative for future studies on isomerization of ketone molecules.

Geometrical Structures and Electronic Properties of Copper-Doped Aluminum Clusters

Using density function theory （DFT）, the Cu-doped Aln （n=1-15） clusters have been stud- ied. The electron affinity, ionization potential, Mulliken population analysis of Cu, mean polarizability, polarizability anisotropy, dipole moments and HOMO-LUMO gaps have also been calculated on the basis of optimized geometries. The results indicate that there is magic numbers in copper-doped aluminum clusters and electronic characteristic depended on the size of clusters. As n=13, the electron affinity and ionization potential of cluster changed more than 0.3 and 0.6 eV respectively, compared with neighborhood clusters.

Adsorption Behavior of CH2 and CH3 on Metal Clusters CUn （n=1-6）

Using density functional theory with generalized gradient approximation and hybrid functional, we studied the properties of energy, charge population, and vibration of CH2 and CH3 adsorbed on Cun （n=1-6） clusters. The results show that the DFT calculation with the hybrid functional matches the experimental results better in both cases. The calculation results indicate that the adsorption of CH2 is stronger than that of CH3. During adsorption, the charges transfer from Cu to CH2 or CH3. The obtained vibrational frequencies for different modes of CH2 and CH3 adsorbed on Cun agree well with the experimental results for the adsorption on Cu（111） surface.

Stable High-Energy Density Super-Atom Clusters of Aluminum Hydride

With the concept of super-atom, first principles calculations propose a new type of super stable cage clusters AlnH3n that are much more energetic stable than the well established clusters, AlnHn＋2. In the new clusters, the aluminum core-frame acts as a super-atom with n vertexes and 2n A1-A1 edges, which allow to adsorb n hydrogen atoms at the top-site and 2n at the bridge-site. Using Al12H36 as the basic unit, stable chain structures, （Al12H36）m, have been constructed following the same connection mechanism as for （A1H3）n linear polymeric structures. Apart from high hydrogen percentage per molecule, calculations have shown that these new clusters possess large heat of formation values and their combustion heat is about 4.8 times of the methane, making them a promising high energy density material.

Resolving multi-orbital effects on high harmonic generation from aligned N2 molecules in linearly and elliptically polarized intense laser fields

We perform an experimental study of the multi-orbital effect on the high-order harmonic generation(HHG) from aligned N_2 molecules in both linearly and elliptically polarized intense laser fields.Measured by a home-built extreme ultraviolet(XUV) flat grating spectrometer with the pump-probe method, the angular distributions of different orders of HHG are obtained, which show distinctive behaviors for harmonics in the plateau and the cut-off regions.The ellipticity dependence of HHG is investigated by aligning the molecular axis parallel or perpendicular to the laser polarization.Our results indicate that both the highest occupied molecular orbital(HOMO) as well as the lower one(HOMO-1) contribute to the HHG of N2 molecules, in either linearly or elliptically polarized intense laser field.The study paves the way for understanding the ultrafast electron dynamics of molecules exposed to an intense laser field.

Photoelectron imaging of resonance-enhanced multiphoton ionization and above-threshold ionization of ammonia molecules in a strong 800-nm laser pulse

In this work, we mainly investigate the NH3 molecular multiphoton ionization process by using the photoelectron velocity map imaging technique. Under the condition of femtosecond laser(wavelength at 800 nm), the photoelectron images are detected. The channel switching and above-threshold ionization(ATI) effect are also confirmed. The kinetic energy spectrum(KES) and the photoelectron angular distributions(PADs) are obtained through the anti-Abel transformation from the original images, and then three ionization channels are confirmed successfully according to the Freeman resonance effect in a relatively low laser intensity region. In the excitation process, the intermediate resonance Rydberg states are C^1 A 1(6 + 2 photons process), B^1 E(6 + 2 photons process) and C^1 A 1(7 + 2 photons process), respectively. At the same time, we also find that the photoelectron angular distributions are independent of laser intensity. In addition, the electrons produced by different processes interfere with each other and they can produce a spider-like structure. We also find ac-Stark movement according to the Stark-shift-induced resonance effect when the laser intensity is relatively high.

Imaging alignment of rotational state-selected CH_3I molecule

We experimentally and numerically investigate CH_3I molecular alignment by using a femtosecond laser and a hexapole. The hexapole provides the single |111〉rotational state condition at 4.5-kV hexapole rod voltage. Based on this single rotational state, an enhanced alignment degree of 0.73 is achieved. Our experimental results are in agreement with the simulation results. We experimentally obtain the ion velocity map images and show the influence of the initial rotational-state population. With the I+ion images and angular distributions at different pump-probe delay time, the alignment and anti-alignment phenomena are further demonstrated. The molecules will be under field-free conditions when the laser effect disappears completely at the full revival time. Our work shows that the quantum control and spatial control on CH_3I molecules can be realized and molecular coordinate frame can be obtained for further molecular experiment.

Softening of C-H Symmetric Stretching Vibrational Modes for CH2 and CH3 Radicals Adsorbed on Cun （n=1-6） Clusters

The properties of C-H vibration softening for CH2 and CHa radicals absorbed on Cun（n=1-6） clusters have been investigated, using the density functional theory with hybrid functional. The results indicate that the absorption of CH2 on Cu clusters is stronger than the case of CH3. The vibrational frequencies of C-H bonding agree with the experimental results obtained for CH2 and CH3 absorbed on Cu（111）. With the increase of cluster size, the softening （Einstein shift） of C-H vibrational modes become stronger.

Dynamic stabilization of atomic ionization in a high-frequency laser field with different initial angular momenta

We investigated the ionization of an atom with different orbital angular momenta in a high-frequency laser field by solving the time-dependent Schr¨odinger equation.The results showed that the ionization stabilization features changed with the relative direction between the angular momentum of the initial state and the vector field of the laser pulse.The ionization mechanism of the atom irradiated by a high frequency was explained by calculating the transition matrix and evolution of the time-dependent wave packet.This study can provide comprehensive understanding to improve atomic nonadiabatic ionization.

Role of rotational state-selected for nonadiabatic alignment： OCS molecules in femtosecond laser fields

Nonadiabatic alignment by intense nonresonant the spatial direction of molecules： By solving the the degree of alignment of the molecules initially laser fields is a versatile technique to manipulate time-dependent SchrSdinger equation numerically in different rotational state are calculated and the results show that the degree of alignment strongly depends on the initial rotational state. Thus, the present study indicates that, for obtaining a high degree of alignment for molecules, appropriate selection of molecular rotational states is necessary.

Controlling continuum wavepacket interference by two-color laser field in over-the-barrier ionization regime

Continuum wavepacket interference is investigated by numerically solving the time-dependent SchrSdinger equation for the interaction of hydrogen atoms with laser fields. The obtained wavepacket evolution indicates that, in the over-the-barrier ionization regime （1016 W/cm2）, the continuum-continuum （CC） interference of ionizing electrons becomes the main process in high- order harmonics generation （HHG）, compared with continuum-bound （CB） transition, as reported by Kohler et al. [Phys. Rev. Lett. 105（20）, 203902 （2010）]. We propose a two-color laser field scheme for controlling the quantum trajectories of ionizing electrons and for extending the CC harmonic energy. As a result, a high energy platform occurs in the HHG spectrum, which entirely originates from the CC harmonics, with a cutoff adjustable by the relative phase of the two-color fields. This provides further understanding of the dynamic feature of atoms and molecules in super intense laser fields and provides an opportunity to image the atomic or molecular potential.