Identification of the physical mechanism of generation of coherent N ₂2 ⁺ emissions in air by femtosecond laser excitation

Recently, amplification of harmonic-seeded radiation generated through femtosecond laser filamentation in air has been observed, giving rise to coherent emissions at wavelengths corresponding to transitions between different vibrational levels of the electronic B2Σ u + and X2Σ g + states of molecular nitrogen ions [Phys. Rev. A. 84, 051802(R) (2011)]. Here, we carry out systematic investigations on its physical mechanism. Our experimental results do not support the speculation that such excellent coherent emissions could originate from nonlinear optical processes such as four-wave mixing or stimulated Raman scattering, leaving stimulated amplification of harmonic seed due to the population inversion generated in molecular nitrogen ions the most likely mechanism.