Lasing of N2+ at 428 nm is studied as a function of the delay dt between two 800 nm ultrashort pumping pulses from a Ti:sapphire laser. This lasing corresponds to a population-inverted transition between levels B2Σu+(0) and X2Σg+(1) of a singly ionized nitrogen molecule. An important erasing of laser emission is observed under pumping with two consecutive pulses separated by large delays −20 ps < dt < +20 ps. From an analysis of the quenching results, we conclude that the mechanism of lasing corresponds to a coherent two-photon amplification scheme. Our results show that a two-photon process can dominate over a population-inverted one-photon amplification.
N2+ lasing action involves the creation, evolution, and radiation of ions in intense laser fields. In this paper, we demonstrate that
N2+ lasing intensity can be enhanced by several times or totally suppressed by controlling the ionic creation and radiation processes through manipulation of the coherent molecular rotational wave packets of
N2 and
N2+ with a pump-control scheme. Our results show that if a weak control pulse arrives at the revival moments of the ionic rotational wave packet, the lasing signal can be notably promoted, which is in contrast to observations in previous studies. Meanwhile, the modulation profiles of the lasing signals caused by molecular alignments of
N2 and
N2+ are analyzed at length, revealing the double roles of the weak control pulse in inducing molecular alignment of
N2 or monitoring the amplification of the
N2+ system by controlling electronic and rotational coherence. Moreover, by performing a Fourier transformation of the delay-dependent
N2+ lasing, the rotational wave-packet information of
N2 and
N2+ is simultaneously retrieved.
We experimentally demonstrate the existence of long-lived coherent polarizations coupling simultaneously ground state X (X2Σg+) to excited states A (A2Πu) and B (B2Σu+) of N2+ inside a plasma created by a short intense laser pulse at 800 nm. This three-level V-scheme arrangement is responsible for a strong optical gain without population inversion at the B–X transition at 391.4 nm. Simulations based on Maxwell-Bloch equations reproduce well the kinetics and the pressure dependence of the gain.
We investigate the formation of rotational coherence of N2+ resonantly interacting with an intense femtosecond laser field by numerical simulations based on a strong-field ionization-coupling model described with the density matrix formalism. The created N2+ system is unique in many aspects: the variable total population within the pump duration due to the intensity-dependent ionization injection, the readily accessible resonance owing to the effect of Stark shift, and the involvement of a few dozen of quantum states. By regarding the N2+ system as an open and non-stationary Λ-type cascaded multi-level system, we quantitatively studied the dependence of rotational coherence in different electronic-vibrational states of N2+ on the alignment angle θ and the pumping intensity. Our simulation results indicate that the quantum coherence between the neighbouring rotational states of J, J+2 in the vibrational state ν=0, 1 of the ground state of N2+ can be changed from a negative to a positive. The significant contribution of rotational coherence to inducing an extra gain or absorption of N2+ air lasing is further verified by solving the Maxwell's propagating equation. The finding provides crucial clues on how to manipulate N2+ lasing by controlling the rotational coherence and paves the way to studying strong-field quantum optics effects such as lasing without inversion and electromagnetically induced transparency in molecular ionic systems.
Nitrogen molecules pumped by intense femtosecond laser pulses give rise to coherent emission in the forward direction at a series of wavelengths, coined “air lasing.” We demonstrate the coherent control of these emissions via a pair of seeding pulses at two different frequencies at low pressures, revealing a coherence transfer through vibrational motion. It is found that the injection of a 427.8 nm (391.4 nm) seeding pulse results in its amplification at the expense of the 391.4 nm (427.8 nm) signal, demonstrating a competition between the two spectral components of the emission from the upper level population. Moreover, when the delay between the seeding and pump pulses is finely tuned, the coherent control of both transitions is observed via the coherence transfer. A microscopic molecular relaxation model reproduces these observations, highlighting the crucial role of electronic and vibrational coherences, as well as their coupling, during the lasing action.
In standard lasers, light amplification requires population inversion between an upper and a lower state to break the reciprocity between absorption and stimulated emission. However, in a medium prepared in a specific superposition state, quantum interference may fully suppress absorption while leaving stimulated emission intact, opening the possibility of lasing without inversion. Here we show that lasing without inversion arises naturally during propagation of intense femtosecond laser pulses in air. It is triggered by the combination of molecular ionization and molecular alignment, both unavoidable in intense light fields. The effect could enable inversionless amplification of broadband radiation in many molecular gases, opening unusual opportunities for remote sensing.