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arXiv:2405.04089 · Physical Review Letters

Bidirectional Cascaded Superfluorescent Lasing in Air Enabled by Resonant Third Harmonic Photon Exchange from Nitrogen to Argon

Zan Nie, Noa Nambu, K. A. Marsh, Daniel Matteo, Chandni Patel, Chaojie Zhang, Yipeng Wu, Stefanos Carlström, Felipe Morales, Serguei Patchkovskii, Olga V. Smirnova, Misha Ivanov, Chan Joshi

Published Aug 7, 2024• 13 citations
arXivHTMLPDF

Abstract

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.

DOI
10.1103/physrevlett.133.063201

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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.
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.
Lasing refers to the generation of highly directional laser-like emission remotely pumped by laser pulses in a medium such as ambient air or a flame.It has been intensively investigated because of its potentials to revolutionize the field of remote sensing.Earlier studies were carried out in flames, where lasing effect has been observed in various radicals, for example H, O, N etc., through two-photon resonant excitation.This scheme was later applied to generate lasing of O and N in ambient air, which can be dramatically improved by predissociation of the air constituents.However, the underlying physical mechanism of two-photon-excited lasing effect is still unsettled although it has been studied for more than one decade.Currently there are three different proposals: (1) Amplified Spontaneous Emission (ASE), in which case population inversion is responsible for optical gain;(2) Superfluorescence (SF), where a macroscopic dipole occurs in the population inverted medium; (3) Both hyper-Raman scattering and four-wave mixing are involved in the generation of lasing emission.Here, we experimentally studied 656 nm lasing emission of atomic hydrogen via two-photon resonant excitation by focusing 125-fs laser pulses of 205-nm wavelength in a methane/oxygen welding flame (see Fig. 1), where hydrogen atoms are naturally present.Lasing occurs in both forward and backward directions, and the forward signal strength is almost one order of magnitude stronger than the backward one.It has been found that the durations of lasing pulses are around 20 ps, and decreases with increasing pump laser energies.Furthermore, the delay of the lasing pulse with respect to the pump pulse decreases with increasing pump energies.These results show high similarities with the behaviors of SF, suggesting that the femtosecond two-photonexcited lasing emission of atomic hydrogen might be SF.
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.
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.
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 observation of multi-THz quantum beats in the amplitude of superfluorescence in pure argon gas, using a time delayed 780-nm probe beam that interrogates the relevant population densities. The superfluorescence is induced by three-photon absorption of an ultrashort 260.5-nm laser pulse that creates coherent and coupled populations in multiple closely spaced 3d3d3d and 5s5s5s Ar levels. Argon pressure and pump laser focusing parameters are seen to modify the frequency of the quantum beats, which is attributed to the absorption of the self-generated, nonresonant third harmonic of the pump from Ar near the zero of the real part of the overlapping linear susceptibilities of the closely spaced 3d3d3d and 5s5s5s excited states. The self-absorption of the phase-matched THG photons creates a coherent population of atoms which acts like an atomic excited state ($3\ensuremath{\omega}$-induced state). We have also observed a new two-step superfluorescent cascade that results from the population redistribution enabled by the 780-nm probe pulse between the $3{d}^{\ensuremath{'}}{[5/2]}_{3}$ and the $3\ensuremath{\omega}$-induced state and gives rise to a previously unknown transition that emits on 1587 nm.