研究目的
Investigating the PFI-ZEKE-photoelectron spectroscopy of N2O using narrow-band VUV laser radiation generated by four-wave mixing in Ar using a KBBF crystal to resolve the rotational structure of vibrational levels of the A+ state of N2O+ and derive improved values of the first two adiabatic ionization energies of N2O.
研究成果
The study successfully resolved the rotational structure of almost all vibrational levels of the A+ state of N2O+ and derived more accurate values for the first two adiabatic ionization energies of N2O. The rotational intensity distributions were found to strongly depend on the vibrational angular momentum of the ionic levels, and the vibrational structure was discussed in terms of effective-Hamiltonian analyses. The use of KBBF crystals was shown to be effective for accessing two-photon resonances of Ar for the generation of intense VUV radiation.
研究不足
The study was limited by the intensity of the VUV laser in certain wave-number ranges, which prevented the measurement of some regions of the spectrum. Additionally, the very weak transitions to certain vibrational levels required the use of supersonically cooled samples, limiting the ability to determine centrifugal distortion constants for these bands.
1：Experimental Design and Method Selection:
The study utilized a new nonlinear optical scheme for generating VUV radiation by sum-frequency mixing in a KBBF crystal, followed by resonance-enhanced four-wave mixing in Ar. This radiation was then used for PFI-ZEKE photoelectron spectroscopy of N2O.
2：2O.
Sample Selection and Data Sources:
2. Sample Selection and Data Sources: A supersonic beam of pure N2O was used for the experiments, with the rotational temperature adjustable between 5 K and room temperature.
3：List of Experimental Equipment and Materials:
The setup included a KBBF crystal for sum-frequency mixing, a pulsed seeded Nd:YAG laser, a single-mode ring dye laser, a double-grating dye laser, and a toroidal dispersion grating for directing the VUV laser beam.
4：Experimental Procedures and Operational Workflow:
The VUV radiation was generated and then used to excite N2O molecules in a supersonic beam. The resulting photoelectrons were detected using a multipulse field-ionization sequence optimized for high-resolution spectra.
5：Data Analysis Methods:
The rotational line positions and intensities were analyzed using a simple orbital-ionization model, and the vibrational term values were calculated using an effective Hamiltonian.
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