Nonsequential double ionization of nonaligned diatomic molecules N2 and O2

Nonsequential double ionization (NSDI) processes of nonaligned diatomic molecules N2 and O2 are studied using the S-matrix theory. Our results show that the NSDI process significantly depends on the molecular symmetry and structure. The ratio of NSDI rate to single ionization rate as a function of the field intensity is obtained. It is found that N2 behaves closely with its companion atom Ar in the ratios over the entire intensity range, while O2 exhibits an obvious suppression effect, which is qualitatively consistent with the experiment.     

Influence of the internuclear vector on ionization of molecules in intense laser field

We theoretically study the influence of the internuclear vector on molecular ionization in linear polarization laser fields through taking O₂, CO₂ as model molecules. We find that the ionization rates of O₂ and CO₂ depend on the molecular orientations. For O₂, the molecular orientation corresponding to the maximum ionization rate is about φ_m = 45^°, which is independent of the laser intensity; while for CO₂, this kind of molecular orientation varies with laser intensity. We also find the ionization suppression of molecule depends on the molecular orientations and the internuclear distance. The ionization suppression easily disappears for molecules with larger internuclear distance.     

Penning ionization electron spectroscopy of CO,HCl, HBr and of triatomic molecules N2O,NO2, CO2, COS and CS2

The energy of electrons released in ionization of di- and triatomic molecules by He (2¹S, 2³S), Ne and Ar (³P_{0, 2}) metastable atoms was measured. Attention was concentrated on the determination of peak shifts and peak form in order to elucidate new features of the mechanism of ionization with respect to ionization of atoms. In ionization by He (2¹S) atoms, asymmetric peak forms and greater shifts towards lower electron energy were found than in ionization by He (2³S) atoms. A tentative explanation for peak shifts in terms of orientation of molecules during the collision and of molecular orbitals involved in ionization was proposed. Effects due to J values of metastable atoms and molecular ions were described. The ionization of electronegative molecules (NO₂) probably takes place already at large particle separation because of mixing with the X⁺ABC^? ionic state which, on recombination, ionizes into X + ABC⁺ + e.     

Molecular orbital study of the interaction of carbon monoxide and carbon dioxide with copper (100)

A molecular orbital study is made of the structures and energy levels of CO and CO₂ on Cu(100). The importance of self-consistency is discussed. CO is found to occupy fourfold indentations, in agreement with the semiempirical results of Doyden and Ertl. The C-surface distance is 1.0 Å and the CO bond stretches less than 0.1 Å. Large models of the surface show convergence of the electronic structure with four CO molecules on a twelve Cu atom cluster model of the surface. At coverages up to c(2 × 2) half monolayer, calculated energy levels match Demuth and Eastman's phase I photoemission spectrum. Phase II, as observed by them, has no analog in the calculations. No evidence is found for CO deviating from perpendicular to the surface when tightly bound. CO₂ is found to adsorb more weakly to the surface. This molecule rests in a μ bridging position, bonded through mixing of Cu d with CO₂ π¹ orbitals. It bends, with an angle of 120°, which is significantly similar to 122° for the ¹B₂ excited state of free CO₂, which has an electron promoted to the π¹ orbital. On the basis of this molecular orbital study, extrapolations to Ni and Zn surfaces and OCS, CS₂, CSe₂ and CTe₂ are made.     

Effects of multi orbital contributions in the angular-dependent ionization of molecules in intense few-cycle laser pulses

We outline the details of our new method to calculate angular-dependent ionization probabilities based on electronic structure theory for diatomic and larger systems. To demonstrate its abilities, we compare our calculations to measured ionization probabilities of the four molecules D₂, N₂, O₂ and CO in the strong-field regime. The calculated angular distributions yield better agreement with the experimental data than those obtained from the widely used MO-ADK theory. For CO the measured angular distributions of ionic fragments indicate contributions to the ionization from both the HOMO and the HOMO-1 orbital, an effect that is addressed by the theory.     

Spectroscopic studies of laser-produced plasmas formed in CO and CO2 using 193, 266, 355, 532 and 1064 nm laser radiation

The wavelength dependence of laser-produced breakdown in air, CO and CO₂ has been studied using the four Nd:YAG harmonics (266 nm, 355 nm, 532 nm and 1064 nm) and the ArF-excimer laser (193 nm). Breakdown thresholds at these wavelengths are reported for air, CO and CO₂. A significant reduction in the breakdown thresholds for both CO and CO₂ is apparent when comparing 193 nm with the four Nd:YAG harmonics. This reduction is attributed to the resonance-enhanced two-photon ionization of metastable carbon atoms generated in the laser focus at the ArF-laser wavelength. In addition to reporting breakdown thresholds, the laser-produced plasmas in CO and CO₂ are characterized in terms of plasma temperatures and electron densities which are measured by time-resolved emission spectroscopy. Electron densities range from 9 × 10¹⁷ cm^–3 to 1 × 10₁₇ cm^–3. Excitation temperatures range from 22 000 K at 0.2 µs to 11 000 K at 2 µs. Ionization temperatures range from 22 000 K at 0.1 µs to 16 000 K at 2 µs. Evidence is presented to indicate that, like ArF-laser-produced plasmas, Nd:YAG-laser-produced plasmas formed in CO and CO₂ are in or near a state of Local Thermodynamic Equilibrium (LTE) soon after their formation.     

不同分子取向下氢分子非次序双电离对核间距的依赖关系

利用三维经典系综模型研究了氢分子非次序双电离对核间距的依赖性.在不同分子取向下,氢分子双电离率随核间距的增大而先增大后减小,在核间距为4a.u.时取最大值.氢分子非次序双电离对核间距的依赖性随分子轴与激光偏振方向间夹角φ的增大而减弱.φ=0时,氢分子非次序双电离包含丰富的相关模式,对核间距有强烈的依赖性φ=π/2时,不同核间距下的相关模式相似,重碰撞在双电离过程中发挥更重要的作用.这些结果表明分子结构对双原子分子非次序双电离有重要影响. 关键词： 非次序双电离 核间距 关联动量分布     

The adsorption sites of CO on Ni(111) as determined by infrared reflection-absorption spectroscopy

The adsorption of CO on Ni(111) has been studied using infrared reflection-absorption spectroscopy combined with LEED, Auger electron spectroscopy, thermal desorption spectroscopy and work function measurements. At low CO coverage (θ = 0.05) CO adsorbs on threefold sites with a strecthing frequency given by ω_CO = 1817 cm^?1. At θ = 0.30 all molecules have shifted to two-fold sites, and θ = 0.50, where a c(4 × 2) structure is observed, ω_CO = 1910 cm^?1. At θ = 0.57, with a (√7/2) × √7/2)R19.1° structure, one quarter of the molecules are adsorbed on top of the nickel atoms with the others in two-fold sites. Molecules bonded on the top sites give rise to a band at 2045 cm^?1. The frequency shift due to dipole-dipole interactions is small compared with the shift resulting from bonding to different crystallographic sites.     

Broadening of a two-photon resonance in a zinc atom in collisions with CO<Subscript>2</Subscript>, CO,and NO molecules

The broadening of a two-photon resonance is studied experimentally at the 4s¹S₀?6s³S₁ transition in a zinc atom upon absorption of two waves with a small detuning from an intermediate state in collisions with CO₂, CO, and NO molecules. The measured absolute values of broadening cross sections greatly exceed gas-kinetic cross sections and are (9.4±2.4, 6.5±1.6, and 3.9±1.0)×10^{? 14}cm² for CO², CO, and NO, respectively. Anomalously large rate constants and cross sections obtained in experiments are explained by the efficient resonance quenching of the excited states of zinc atoms in collisions with molecules accompanied by transfer of the energy of excited atoms to vibrational-rotational degrees of freedom of molecules.     

Infrared spectra of the Kr—CO and Xe—CO van der Waals complexes

The infrared spectra of the weakly bound complexes Kr—CO and Xe—CO have been studied in the region of the CO stretching vibration (4.7 μm) using a high-resolution tuneable diode laser probe. The complexes were observed in a long path (200 m) low temperature (76 K) gas cell (Kr—CO) and in a pulsed supersonic jet expansion (Kr—CO and Xe—CO). Previous long path cell measurements on these complexes at lower resolution analysed only the K = 0 and 1 stacks of rotational levels in the ground intermolecular vibrational state. The new data extend up to K = 3 (Xe—CO) or 4 (Kr—CO), and also include K = 0 and 1 stacks in the excited bending state, ν₂ = 1. The bending frequencies for Kr—CO and Xe—CO (in the ν_co = 1 upper state) were determined to be 13.156cm_?1 and 13.794cm^?1, respectively. Detailed molecular parameters were determined to describe the rotational energy levels of each complex using a simple empirical Hamiltonian. These results enable parameters to be compared for the entire series of rare gas—carbon monoxide complexes, from He—CO to Xe—CO. Also they will guide the future development and evaluation of accurate intermolecular potential energy surfaces for Kr—CO and Xe—CO.