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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.
We investigate the generation of broadband terahertz (THz) pulses with phase singularity from air plasmas created by fundamental and second harmonic laser pulses. We show that when the second harmonic beam carries a vortex charge, the THz beam acquir
We experimentally demonstrate generation of strong narrow-bandwidth emissions with excellent coherent properties at ~391 nm and ~428 nm from molecular ions of nitrogen inside a femtosecond filament in air by an orthogonally polarized two-color driver
We experimentally demonstrate energy exchange between a delay-tuned femtosecond beam and two delay-fixed ones as they spatiotemporally overlapped and experienced filamentation in air. The energy exchange process in the relative time delay is dramatic
We demonstrate experimentally the resonant excitation of plasma waves by trains of laser pulses. We also take an important first step to achieving an energy recovery plasma accelerator by showing that unused wakefield energy can be removed by an out-
The use of strong-field (i.e. intensities in excess of 10^13 Wcm-2) few-cycle ultrafast (durations of 10 femtoseconds or less) laser pulses to create, manipulate and image vibrational wavepackets is investigated. Quasi-classical modelling of the init