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.
The ionization processes of NH3 molecule are studied by photoelectron velocity map imaging technique in a linearly polarized 400-nm femtosecond laser field. The two-dimensional photoelectron images from ammonia molecules under different laser intensities are obtained. In the slow electron region, the values of kinetic energy of photoelectrons corresponding to peaks 1, 2, 3, and 4 are 0.27, 0.86, 1.16, and 1.6 eV, respectively. With both the kinetic energy and angular distribution of photoelectrons from NH3 molecules, we can confirm that the two-photon excited intermediate Rydberg state is A^1 A2" (v2'=3) state for photoelectron peaks 2, 3, 4, and the three peaks are marked as 1223 (2 + 2), 1123 (2 + 2), and 1023 (2 + 2) multi-photon processes, respectively. Then, peak 1 is found by adding a hexapole between the source chamber and the detection chamber to realize the rotational state selection and beam focusing. Peak 1 is labeled as the 1323 (3 + 1) multi-photon process through the intermediate Rydberg state E^1A1'. The phenomena of channel switching are found in the slow electron kinetic energy distributions. Our calculations and experimental results indicate that the stretching vibrational mode of ammonia molecules varies with channels, while the umbrella vibration does not. In addition, we consider and discuss the ac-Stark effect in a strong laser field. Peaks 5 and 6 are marked as (2 + 2 + 1) and (2 + 2 + 2) above threshold ionization processes in the fast electron region.
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.
The above-threshold ionization process of ammonia molecules induced by a femtosecond laser field at 800 nm is studied in the intensity range from 1.6×10^(13) to 5.7×10^(13)W/cm^(2).Channel switching under different laser intensities is observed and identified in the photoelectron kinetic energy spectra of ammonia.Based on the photoelectron kinetic energy distributions and the photoelectron angular distributions,the characteristic peaks observed are exclusively assigned to the multiphoton resonance through certain intermediate states,followed by multiphoton above-threshold ionization.
