Search

We present the results of a combined experimental and numerical study on strong-field ionisation of acetylene performed with the aim of identifying the mechanism behind the previously reported surprisingly large multi-electron ionisation probabilities of polyatomic molecules. Using coincidence momentum imaging techniques and time-dependent density functional simulations, we show that the reported efficient ionisation is due to the combined action of a significant geometrically induced energy upshift of the most relevant valence orbitals as the C–H distance stretches beyond about two times the equilibrium distance, and a strong increase in the coupling between multiple molecular orbitals concomitant with this stretch motion. The identified enhanced ionisation mechanism, which we refer to as EIC-MOUSE, is only effective for molecules aligned close to parallel to the laser polarisation direction, and is inhibited for perpendicularly aligned molecules because of a suppression of the C–H stretch motion during the onset of ionisation. [ABSTRACT FROM AUTHOR]

We present the theoretical model for a single-pass, discharge-type standoff nitrogen laser initiated by a femtosecond filament in nitrogen gas. The model is based on the numerical solution of the kinetic equation for the electron energy distribution function self-consistently with balance equations for nitrogen species and laser equations. We identify the kinetic mechanisms responsible for a buildup of population inversion in the filament afterglow plasma and determine the dependence of population inversion density and the parameters of nitrogen lasing at a 337 nm wavelength corresponding to the transition between the C3Πu (v = 0) excited and the X1Σg (v = 0) ground electronic states in a nitrogen molecule on the polarization and wavelength of the driver laser pulse used to produce the filament. We show that population inversion is achieved on an ultrafast time scale of ≈10 ps and decays within the time: <100 ps. We derive the low-signal gain 2.2 cm−1 for lasing from a circularly polarized 0.8 μm near-IR filament and 0.16 cm−1 for a linearly polarized 4 μm mid-IR filament. The results of the numerical simulations demonstrate good quantitative agreement with the experimental measurements. [ABSTRACT FROM AUTHOR]