Ultrashort long-wave infrared (LWIR) laser pulses can resonantly excite vibrations in N2 and O2 through a two-photon transition. The absorptive, vibrational component of the ultrafast optical nonlinearity grows in time, starting smaller than, but quickly surpassing, the electronic, rotational, and vibrational refractive components. The growth of the vibrational component results in a novel mechanism of 3rd harmonic generation, providing an additional two-photon excitation channel, fundamental + 3rd harmonic. The original and emergent two-photon excitations drive the resonance exactly out of phase, causing spatial decay of the absorptive, vibrational nonlinearity. This nearly eliminates two-photon vibrational absorption. Here we present simulations and analytical calculations demonstrating how these processes modify the ultrafast optical nonlinearity in air. The results reveal nonlinear optical phenomena unique to the LWIR regime of ultrashort pulse propagation in atmosphere.
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