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We use time- and frequency-resolved measurements of self-focusing and self-defocusing of 4.3-\ensuremath{\mu}m radiation in ${\mathrm{CO}}_{2}$ gas to study the resonant nonlinear optical response in the vicinity of individual rovibrational lines. Measurements over a range of lines on the $4P$ and $4R$ branch of the 000-001 transition indicate that the nonlinear response of ${\mathrm{CO}}_{2}$ is strongly affected by power broadening, resulting in a sign reversal of the nonlinearity as compared to that of a saturable two-level system.

physical review. a/physical review, a

Resonant nonlinear refraction of 4.3-μm light in <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"><mml:mrow><mml:msub><mml:mi mathvariant="normal">CO</mml:mi><mml:mn>2</mml:mn></mml:msub></mml:mrow></mml:math> gas

Resonant nonlinear refraction of 4.3-μm light in CO2 gas