Electronic State Population Dynamics upon Ultrafast Strong Field Ionization and Fragmentation of Molecular Nitrogen

Air lasing from single ionized N_{2}^{+} molecules induced by laser filamentation in air has been intensively investigated and the mechanisms responsible for lasing are currently highly debated. We use ultrafast nitrogen K-edge spectroscopy to follow the strong field ionization and fragmentation dynamics of N_{2} upon interaction with an ultrashort 800 nm laser pulse. Using probe pulses generated by extreme high-order harmonic generation, we observe transitions indicative of the formation of the electronic ground X^{2}Σ_{g}^{+}, first excited A^{2}Π_{u}, and second excited B^{2}Σ_{u}^{+} states of N_{2}^{+} on femtosecond timescales, from which we can quantitatively determine the time-dependent electronic state population distribution dynamics of N_{2}^{+}. Our results show a remarkably low population of the A^{2}Π_{u} state, and nearly equal populations of the X^{2}Σ_{g}^{+} and B^{2}Σ_{u}^{+} states. In addition, we observe fragmentation of N_{2}^{+} into N and N^{+} on a timescale of several tens of picoseconds that we assign to significant collisional dynamics in the plasma, resulting in dissociative excitation of N_{2}^{+}.