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Optica

Coherent control of the multiple wavelength lasing of ${\rm N}_2^ +$: coherence transfer and beyond

Xiang Zhang, Qi Lu, Zhedong Zhang, Zhengquan Fan, Dongjie Zhou, Qingqing Liang, Luqi Yuan, Songlin Zhuang, Konstantin E. Dorfman, Yi Liu

Published Mar 29, 2021• 32 citations
Publisher

Abstract

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.

DOI
10.1364/optica.417804

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Coherent control of the multiple wavelength lasing of N2+{\rm N}_2^ +N2+​: coherence transfer and beyond
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.
Singly ionized nitrogen molecules in ambient air pumped by 800 nm femtosecond laser give rise to superradiant emission. Here, we study this superradiance by injecting a pair of resonant seeding pulses at different intensity ratios inside the nitrogen gas plasma. Strong modulation of the 391.4 nm superradiant emission with a period of 1.3 fs is observed when the delay between the two seeding pulses is finely tuned. The modulation contrast is increased and then decreased with the delay time when the second seed pulse is stronger than the first one, and the maximum modulation contrast occurs at longer delay time when the second seeding pulse is stronger. This reveals the increase of the macroscopic polarization with time after the seeding pulse. Moreover, these observations provide a new level of control on the "air lasing" based on nitrogen ions, which can find potential applications in optical remote sensing.
We report a combined theoretical and experimental investigation on the unambiguous role of electronic coherence underlying the generation of laserlike coherent emission from N2+{{\mathrm{N}}_{2}}^{+}N2​+ ions launched in a strong laser field. The coherence manifests itself by giving rise to a dramatic enhancement of N2+{{\mathrm{N}}_{2}}^{+}N2​+ laserlike radiation with two temporally separated pump laser pulses centered at 800- and 1580-nm wavelengths, respectively. We further show that coherent control of N2+{{\mathrm{N}}_{2}}^{+}N2​+ lasing in a subfemtosecond timescale can be achieved by replacing the single 800-nm laser pulse with a pair of 800-nm laser pulses of adjustable time delay. The experimental results are well reproduced in theory using a three-level quantum model of N2+{{\mathrm{N}}_{2}}^{+}N2​+ ions under the density matrix representation.
Multiple gain routes complicate the amplification behaviors of N2+ lasing. A direct comparison of the amplification processes of various lasing lines of N2+ is still lacking to date, mainly because the efficient generation of different lasing lines requires different experimental conditions. In this work, to overcome the limitation, we use an intense polarization-modulated femtosecond laser pulse to simultaneously produce high-intensity N2+ lasing signals at 391 nm and 428 nm, permitting us readily performing their time-domain characterizations. Our results show that the primary amplification of 428-nm lasing is always retarded by a few picoseconds with respect to the probe pulse while the amplification of 391-nm lasing can be basically completed within the probe pulse duration at a relatively high gas pressure, and besides, the time duration of the former sustains several times longer than that of the latter. These observations indicate the non-negligible contribution of the initial electronic coherence established by the pump laser, apart from the external triggering pulse. For the 391-nm lasing, the seed amplification and superradiance can fiercely interplay within the probe pulse duration. However, for the 428-nm lasing, its amplification is in essence Raman-assisted superfluorescence due to the lacking of the initial electronic coherence and a direct triggering pulse. Our findings not only shed light on the physics of N2+ lasing but also promote the relevant studies on the collective emissions in the cascaded multi-level molecular ion system.
Air lasing induced by laser filamentation opens a new route for research on atmospheric molecular physics and remote sensing. The generation of air lasing is composed of two processes, i.e., building up optical gain of air molecules in femtosecond time scale and emitting coherent radiation in picosecond time scale. Here, we focus on the emission mechanisms of N 2 + air lasing and reveal, by examining the intensities and temporal profiles of N 2 + lasing at 391 nm generated respectively in a time-varying polarization-modulated and a linearly polarized pump laser field under different nitrogen gas pressures, that the N 2 + lasing can emit through either triggered super-radiance or seed amplification. We find that the two pressure-sensitive factors, i.e., the dipole dephasing time T 2 and the population inversion density n , determine which of these two mechanisms dominates the N 2 + lasing emission process, enabling manipulation of the transition from triggered super-radiance to seed amplification or vice versa. Our findings clarify the emission mechanism of N 2 + lasing under different pressures and provide a deeper understanding of N 2 + air lasing not only in the establishment of optical gain but also in the lasing emission process.
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.
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.