Ionization and dissociation of linear triatomic molecules, carbon dioxide, are studied in 50-fs 800-nm strong laser fields using time-of-flight mass spectrometer. The yields of double charged ions CO2^2+ and various fragment ions(CO^+,O^n+, and C^n+(n = 1, 2)) are measured as a function of ellipticity of laser polarization in the intensity range from 5.0 ×10^13W/cm2 to 6.0 × 10^14W/cm^2. The results demonstrate that non-sequential double ionization, which is induced by laser-driven electron recollision, dominates double ionization of CO2 in the strong IR laser field with intensity lower than2.0 × 10^14W/cm^2. The electron recollision could also have contribution in strong-field multiple ionization and formation of fragments of CO2 molecules. The present study indicates that the intensity and ellipticity dependence of ions yields can be used to probe the complex dynamics of strong-field ionization/dissociation of polyatomic molecules.
Ionizations and fragmentations of benzene, methylbenzene, and chlorobenzene are studied in linearly polarized 50-fs, 800-nm and 400-nm strong laser fields using a time-of-flight mass spectrometer. It is shown that at low laser intensity, the parent ions are dominant for any one of the molecules in an 800-nm strong laser field, while extensive fragmentation is observed in a 400-nm laser field, which can be understood by the resonant photon absorption of molecular cations. The ratio of the yield of the parent ion to the yield of the total ion for each molecule is measured as a function of laser intensity in a range from 1.0 × 1013 W/cm2 to 4.0 × 1014 W/cm2, in either the 800-nm or 400-nm laser field. The results show that the fragmentation of the aromatic molecules increases significantly as the laser intensity is increased. Possible mechanisms for fragmentation in strong laser fields are discussed. Finally, the saturation intensity of ionization of the titled molecules is also determined.
The 18 A-S states correlated to the lowest dissociation limit of SiTe were calculated by using a high-level multirefer-ence configuration interaction (MRCI) method, including scalar relativistic and spin-orbit coupling effects. Based on the calculated potential energy curves, the spectroscopic constants of bound states were determined, which are well consistent with previous experimental results. The spin-orbit matrix elements between the A-S states were computed, which lead to an in-deoth understanding, of oerturbations on the electronic state a^3∏. Finally. the transition dioole moments of allowed transitionsA^1∏-X^1∑^+,E^1∑^+-X^1∑^+,a^3∏-d^3△,a^3∏-d^3△,a^∏-a′^3∑^+,a^3∏-e^3∑^-,and the radiative lifetimes of A^1∏,E^1∑^+,and a^3∏ were evaluated.
Rydberg state excitations of neutral nitric oxide molecules are studied in strong ultraviolet (UV) and near-infra-red (IR) laser fields using a linear time-of-flight (TOF) mass spectrometer with the pulsed electronic field ionization method. The yield of Rydberg molecules is measured as a function of laser intensity and ellipticity, and the results in UV laser fields are compared with those in near-IR laser fields. The present study provides the first experimental evidence of neutral Rydberg molecules surviving in a strong laser field. The results indicate that a rescattering-after-tunneling process is the main contribution to the formation of Rydberg molecules in strong near-IR laser fields, while multi-photon excitation may play an important role in the strong UV laser fields.
Carbon monosulfide molecular ion (CS+), which plays an important role in various research fields, has long been attracting much interest. Because of the unstable and transient nature of CS+, its electronic states have not been well investigated. In this paper, the electronic states of CS+ are studied by employing the internally contracted multireference configuration interaction method, and taking into account relativistic effects (scalar plus spin–orbit coupling). The spin–orbit coupling effects are considered via the state-interacting method with the full Breit–Pauli Hamiltonian. The potential energy curves of 18 Λ–S states correlated with the two lowest dissociation limits of CS+ molecular ion are calculated, and those of 10 lowest Ω states generated from the 6 lowest Λ–S states are also worked out. The spectroscopic constants of the bound states are evaluated, and they are in good agreement with available experimental results and theoretical values. With the aid of analysis of Λ–S composition of Ω states at different bond lengths, the avoided crossing phenomena in the electronic states of CS+ are illuminated. Finally, the single ionization spectra of CS (X1Σ+) populating the CS+(X2Σ1/2+, A2Π3/2, A2Π1/2, and B2Σ1/2+) states are simulated. The vertical ionization potentials for X2Σ1/2+, A2Π3/2, A2Π1/2, and B2Σ1/2+ states are calculated to be 11.257, 12.787, 12.827, and 15.860 eV, respectively, which are accurate compared with previous experimental results, within an error margin of 0.08 eV^0.2 eV.