Perturbative nearly-degenerate four-wave mixing lineshapes in gases
Nearly-degenerate four-wave mixing (NDFWM) spectroscopy and the closely related tunable-laser-induced grating spectroscopies have proved to be valuable tools in the study of nonlinear optical interactions. The NDFWM spectral lineshape provides information concerning the lifetimes, and therefore the identities, of multiphoton scattering mechanisms. In addition to the great number of investigations in liquids and solids, considerable research has focused on wave-mixing in resonant atomic gases for phase conjugation applications. Although many special cases have been discussed, general expressions that include the effects of molecular motion for the NDFWM lineshape in gases have not been previously reported. The present study is motivated by an interest in understanding the mechanisms contributing to degenerate four-wave mixing (DFWM) spectroscopy in molecular gases for application to combustion and chemical physics research. In this study, expressions for the NDFWM lineshape have been developed for nearly forward- and counter-propagating collinear pump-beam geometries. The lineshapes have been derived by applying the velocity integration methods used by Lam and Abrams for the phase-conjugate DFWM to the perturbation-theory expressions developed by Tretout, et al. for resonance coherent anti-Stokes Raman spectroscopy. The resultant expressions thus include the effects of molecular degeneracy on the polarization characteristics of {Chi}.
- Research Organization:
- Sandia National Labs., Livermore, CA (United States)
- Sponsoring Organization:
- USDOE, Washington, DC (United States)
- DOE Contract Number:
- AC04-76DP00789
- OSTI ID:
- 10109416
- Report Number(s):
- SAND--93-8401C; CONF-930151--2; ON: DE93002673
- Country of Publication:
- United States
- Language:
- English
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Related Subjects
400102
664400
74 ATOMIC AND MOLECULAR PHYSICS
CHEMICAL AND SPECTRAL PROCEDURES
COMBUSTION
EXPERIMENTALLY DERIVED INFORMATION ON ATOMIC AND MOLECULAR PROPERTIES
FLAMES
FREQUENCY MIXING
GASES
LASER SPECTROSCOPY
LINE WIDTHS
MULTI-PHOTON PROCESSES
SCATTERING
SPECTROSCOPY