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Physical Review A

Lasing dynamics of neutral nitrogen molecules in femtosecond filaments

Pengji Ding, Eduardo Oliva, Aurélien Houard, A. Mysyrowicz, Yi Liu

Published Oct 17, 2016• 39 citations
Publisher

Abstract

We investigate the dynamics of cavity-free lasing from neutral nitrogen molecules in femtosecond laser filaments. An important difference of intensity and temporal duration is observed between backward and forward lasing, in both amplified spontaneous emission and seed-amplification regimes. Numerical simulations based on a nonadiabatic Maxwell-Bloch model reproduce well the observations, and attribute these differences to the finite gain lifetime and the traveling excitation nature of this gas laser.

DOI
10.1103/physreva.94.043824

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We investigate the dynamics of cavity-free lasing from neutral nitrogen molecules in femtosecond laser filaments. An important difference of intensity and temporal duration is observed between backward and forward lasing, in both amplified spontaneous emission and seed-amplification regimes. Numerical simulations based on a nonadiabatic Maxwell-Bloch model reproduce well the observations, and attribute these differences to the finite gain lifetime and the traveling excitation nature of this gas laser.
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Nitrogen ions pumped by intense femtosecond laser pulses present an optical gain at 391.4 nm, evident by energy amplification of an injected resonant seeding pulse. We report a time-resolved measurement of the amplification process with seeding pulses having varying intensities. It is found that the amplification factor depends on the intensity of the seeding pulse and the effective temporal window for the optical gain becomes longer by applying more intense seeding pulses. These two features are in sharp contrast with classic pump-probe experiments, pinpointing the crucial role of macroscopic coherence and its dynamics during the lasing process. We further measure the temporal profile of the amplified emission for seeding pulse injected at different time delays. A complicated temporal behavior is observed, which highlights the nature of the superfluorescence.
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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.
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.
Nitrogen molecules are ionized when an intense 800-nm femtosecond laser propagates through a nitrogen gas cell. We experimentally probe the relative population in different vibrational states and electronic states of ionized nitrogen molecules by using an external seed with various wavelengths. It is found that the seed is amplified or attenuated depending on its wavelength when the seed passes through the ionized nitrogen gas. Through measuring the temporal profile, the amplified emission is attributed to the seed-triggered superradiance. Combining with theoretical calculation, our results demonstrate that both vibrational and electronic excitation occurs for ionized nitrogen molecules in 800-nm femtosecond laser fields. The population inversion is built between some quantum states of ionized nitrogen molecules, through which the seed-triggered superradiance is achieved.