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Conference on Lasers and Electro-Optics Pacific Rim (CLEO-PR)

Remote lasing in air driven by strong laser field: Lasing or nonlinear frequency conversion?

Jielei Ni, W. Chu, Jinping Yao, Bin Zeng, Huailiang Xu, S. L. Chin, Ya Cheng, Zhenzhu Xu

Published Jun 1, 2013• 0 citations
Publisher

Abstract

We demonstrated systematic investigations on the mechanism of remote coherent N2+emission in air using a pump-probe configuration. Our experimental results suggest lasing action based on instantaneous population inversion is the most likely mechanism.
DOI
10.1109/cleopr.2013.6600313

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Air lasing is a concept that refers to remote no-cavity (mirrorless) optical amplification in ambient air with the air constituents as the gain media. Due to the high potential of air lasing in view of applications in atmospheric sensing, a variety of pumping schemes have been proposed so far for building up population-inverted gain media in air and producing forward and/or backward directional lasing emissions. This review paper presents an overview of recent advances in the experimental observations and physical understanding of air lasing in various pumping schemes of air molecules by intense laser fields. Special emphasis is given to the strong-field-induced N 2 + air lasing, the mechanism of which is currently still in a hot debate.
A cavity-free laser in the sky could lead to revolutionary improvements in optical remote sensing for atmospheric science. Abundant in air, nitrogen molecules are prime candidates as an active medium for such a laser. Nitrogen molecules, either neutral or singly ionized, exhibit a significant optical gain in the UV regime when pumped by an intense femtosecond laser. Despite numerous works, the physical origin of this lasing is still not understood. Here we offer a consistent interpretation of all experimental facts by introducing a concept drawn from the field of quantum optics: transient lasing without inversion. Our experiments and simulations identify the crucial role of macroscopic coherence, instead of population inversion, in the nitrogen ions lasing system. Manipulating the macroscopic coherence provides a new level of control over nitrogen air lasing and offers new perspectives for the generation of very short wavelength laser where population inversion is difficult to achieve.
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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.
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.
Cavity-free lasing in atmospheric air has stimulated intense research toward a fundamental understanding of underlying physical mechanisms. In this Letter, we identify a new mechanism-a third-harmonic photon mediated resonant energy transfer pathway leading to population inversion in argon via an initial three-photon excitation of nitrogen molecules irradiated by intense 261 nm pulses-that enables bidirectional two-color cascaded lasing in atmospheric air. By making pump-probe measurements, we conclusively show that such cascaded lasing results from superfluorescence rather than amplified spontaneous emission. Such cascaded lasing with the capability of producing bidirectional multicolor coherent pulses opens additional possibilities for remote sensing applications.