Saturation effects in gas-phase degenerate four-wave mixing spectroscopy: nonperturbative calculations
Abstract
Saturation effects in gas-phase degenerate four-wave mixing (DFWM) are investigated for conditions of interest for diagnostic applications in flames and plasmas. In particular, the case in which Doppler and collisional broadening are comparable, as is often the case for flame species such as NO and OH, is investigated. DFWM line shapes and signal intensities are calculated nonperturbatively and compared with high-resolution laser measurements. In the nonperturbative calculations the time-dependent density-matrix equations for a two-level system interacting with three laser fields are integrated directly on a grid of spatial locations along the phase-matching axis. The electric-field amplitude for the DFWM signal is determined by multiplying the time-varying, laser-induced polarization at each grid point by the appropriate phase factor and then by summing over all grid points. The calculations are in excellent agreement with measurements of DFWM line shapes and signal intensities for NO in a buffer gas of He over a wide range of He pressure. Under saturation conditions the pressure dependence of the DFWM signal is reduced greatly compared with the unsaturated case. The signal level is still dependent on the ratio of pure dephasing to quenching collisions, even for saturation conditions. From the standpoint of minimal dependence on collisional processes it appears that operation with pump-laser intensities approximately equal to the saturation intensity is optimal. The dependence of the DFWM line shape and signal intensity on the ratio of probe to pump-laser intensity is also investigated.
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FWM with optical lasers is an important technique that can be used in fields as diverse as combustion science and molecular spectroscopy.
“FWM with optical lasers is an important technique, which can be used in fields as diverse as combustion science [70] and molecular spectroscopy [71].”
From Roadmap of ultrafast x-ray atomic and molecular physics (2018) · cites this paper as [70]
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Roadmap of ultrafast x-ray atomic and molecular physics
Young, L., Ueda, K., Gühr, M., Bucksbaum, P. H., Simon, M., Mukamel, S., Rohringer, N., Prince, K. C., Masciovecchio, C., Meyer, M., et al. (2018) · Journal of Physics B: Atomic, Molecular and Optical Physics · doi:10.1088/1361-6455/aa9735 · Cited by 337 · see citing works
Okazaki, A., Ebata, T., & Mikami, N. (1997) · The Journal of Chemical Physics · doi:10.1063/1.475168 · Cited by 47 · see citing works
- Authors
- Lucht, R. P., Farrow, R. L., & Rakestraw, D. J.
- Affiliations
- Sandia National Laboratories California (US)
- Venue
- Journal of the Optical Society of America B
- Publisher
- Optica Publishing Group
- Published
- 1993-09-01
- Volume
- 10
- Issue
- 9
- Pages
- 1508
- ISSN
- 0740-3224 (ISSN-L)
- 1520-8540
- OpenAlex
- W2110318898
- Cited by
- 75
- References
- 33
- Citations by year
- 2020: 1 · 2018: 1 · 2016: 3 · 2013: 2
- FWCI
- 5.88
- Type
- journal article
- Language
- en
- Open access
- closed
- Locations
- Journal of the Optical Society of America B (publishedVersion)
- Topics
- Physical Sciences › Chemistry › Spectroscopy › Spectroscopy and Laser Applications
- Physical Sciences › Physics and Astronomy › Atomic and Molecular Physics, and Optics › Laser-Matter Interactions and Applications
- Physical Sciences › Physics and Astronomy › Atomic and Molecular Physics, and Optics › Quantum optics and atomic interactions
- Keywords
- degenerate four-wave mixing, saturation effects, non-perturbative calculations, time-dependent density matrix, two-level system, Doppler broadening, pressure broadening, nitric oxide, OH, flame diagnostics, plasma diagnostics, pressure dependence, pure dephasing, line shape, signal intensity, phase matching
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