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Title: Raman spectroscopic studies of isotopic diatomic molecules and a technique for measuring stable isotope ratios using Raman scattering. [Cross sections]

Technical Report ·
DOI:https://doi.org/10.2172/7358154· OSTI ID:7358154

A method for measuring stable isotope ratios using Raman scattering has been developed. This method consists of simultaneously counting photons scattered out of a high-intensity laser beam by different isotopically-substituted molecules. A number of studies of isotopic diatomic molecules have been made. The Q-branches of the Raman spectra of the isotopic molecules /sup 14/N/sup 15/N and /sup 16/O/sup 18/O were observed at natural abundance in nitrogen and oxygen samples. Comparison of the ratios of the intensities of the Q-branches of the major nitrogen and oxygen isotopic molecules with mass spectrometric determinations of the isotopic compositions yielded scattering cross sections of /sup 14/N/sup 15/N relative to /sup 14/N/sup 14/N and /sup 16/O/sup 18/O relative to /sup 16/O/sup 16/O. These cross section ratios differ from unity, a difference which can be explained by considering nuclear mass effects on the Franck-Condon factors of the molecular transitions. The measured intensities of the /sup 14/N/sup 15/N and /sup 16/O/sup 18/O Q-branches provided the baseline data needed to make the previously-mentioned extrapolation. High-resolution (approximately 0.15 cm/sup -1/) spectra of the Q-branches of /sup 14/N/sup 14/N and /sup 16/O/sup 16/O yielded a direct determination of ..cap alpha../sub e/ (the difference between the rotational constant in the ground and first excited vibrational states) for these molecules. The measured values are in excellent agreement with those obtained by other means. Complete Raman spectra (pure rotation, rotation-vibration, and high-resolution Q-branch) were obtained on a sample of pure /sup 18/O/sup 18/O. Analysis of this data yielded the molecular parameters: the equilibrium internuclear separation r/sub e/, the moment of inertia I/sub e/, and the energy parameters ..cap alpha../sub e/, B/sub e/, and ..delta..G/sub /sup 1///sub 2//. These are in good agreement with data obtained by microwave spectroscopy.

Research Organization:
Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
DOE Contract Number:
W-7405-ENG-48
OSTI ID:
7358154
Report Number(s):
UCRL-52077; TRN: 76-019040
Resource Relation:
Other Information: Thesis
Country of Publication:
United States
Language:
English