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arXiv:2205.07405 · Ultrafast Science

Multiple-Photon Resonance Enabled Quantum Interference in Emission Spectroscopy of N2+

Xiang Zhang, Qi Lu, Yalei Zhu, Jing Zhao, Rostyslav Danylo, Liang Xu, Mingwei Lei, Hongbing Jiang, Chengyin Wu, Zhedong Zhang, Aurélien Houard, Vladimir T Tikhonchuk, A. Mysyrowicz, Qihuang Gong, Songlin Zhuang, Zengxiu Zhao, Yi Liu

Published Dec 4, 2023• 16 citations
arXivHTMLPDF

Abstract

Quantum interference occurs frequently in the interaction of laser radiation with materials, leading to a series of fascinating effects such as lasing without inversion, electromagnetically induced transparency, Fano resonance, etc. Such quantum interference effects are mostly enabled by single-photon resonance with transitions in the matter, regardless of how many optical frequencies are involved. Here, we report on quantum interference driven by multiple photons in the emission spectroscopy of nitrogen ions that are resonantly pumped by ultrafast infrared laser pulses. In the spectral domain, Fano resonance is observed in the emission spectrum, where a laser-assisted dynamic Stark effect creates the continuum. In the time domain, the fast-evolving emission is measured, revealing the nature of free-induction decay arising from quantum radiation and molecular cooperativity. These findings clarify the mechanism of coherent emission of nitrogen ions pumped with mid-infrared pump laser and are found to be universal. The present work opens a route to explore the important role of quantum interference during the interaction of intense laser pulses with materials near multiple photon resonance.

DOI
10.34133/ultrafastscience.0051

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Quantum interference occurs frequently in the interaction of laser radiation with materials, leading to a series of fascinating effects such as lasing without inversion, electromagnetically induced transparency, Fano resonance, etc. Such quantum interference effects are mostly enabled by single-photon resonance with transitions in the matter, regardless of how many optical frequencies are involved. Here, we report on quantum interference driven by multiple photons in the emission spectroscopy of nitrogen ions that are resonantly pumped by ultrafast infrared laser pulses. In the spectral domain, Fano resonance is observed in the emission spectrum, where a laser-assisted dynamic Stark effect creates the continuum. In the time domain, the fast-evolving emission is measured, revealing the nature of free-induction decay arising from quantum radiation and molecular cooperativity. These findings clarify the mechanism of coherent emission of nitrogen ions pumped with mid-infrared pump laser and are found to be universal. The present work opens a route to explore the important role of quantum interference during the interaction of intense laser pulses with materials near multiple photon resonance.
We report on an investigation of simultaneous generation of several narrow-bandwidth laser-like coherent emissions from nitrogen molecular ions ( ) produced in intense mid-infrared laser fields. With systematic examinations on the dependences of coherent emissions on gas pressure as well as several laser parameters including laser intensity, polarization and wavelength of the pump laser pulses, we reveal that the multiple coherent emission lines generated in originate from a series of nonlinear processes beginning with four-wave mixing, followed with stimulated Raman scattering. Our analyses further show that the observed nonlinear processes are greatly enhanced at the resonant wavelengths, giving rise to high conversion efficiencies from the infrared pump laser pulses to the coherent emission lines near the transition wavelengths between the different vibrational energy levels of ground X and that of the excited B states.
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We investigate the pump wavelength dependence of population inversion in a nitrogen ion when nitrogen gas is irradiated by a femtosecond laser pulse in the wavelength range from ultraviolet to near-infrared. It is found that the population inversions corresponding to the transitions at 391 and 428 nm are very sensitive to the laser wavelength, with extreme values near 400 and 1000 nm. For the ultraviolet pump, the population inversions for 391 and 428 nm transitions occur at different wavelengths: a maximum inversion for the first corresponds to a minimum for the second. This is attributed to the near-resonance single-photon transition combined with the Raman process. A significantly stronger inversion is observed for the near-infrared laser, with the maximum depending on the laser intensity, ascribed to the ac Stark effect. The Floquet theory confirms this conclusion and reveals that the three-photon transition assisted by the strong laser field leads to this enhanced population inversion. This study provides the optimal conditions for air lasing based on ionic transitions of nitrogen molecules.
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.
Molecular ions, produced via ultrafast ionization, can be quantum emitters with the aid of resonant electronic couplings, which makes them the ideal candidates to study strong-field quantum optics. In this work, we experimentally and numerically investigate the necessary condition for observing a collective emission arising from macroscopic quantum polarization in a population-inverted N 2 + gain system, uncovering how the individual ionic emitters proceed into a coherent collection within hundreds of femtoseconds. Our results show that for a relatively high-gain case, the collective emission behaviors can be readily initiated for all the employed triggering pulse area. However, for a low-gain case, the superradiant amplification is quenched since the building time of macroscopic interionic quantum coherence exceeds the dipole dephasing time, in which situation the seed amplification and free induction decay play an essential role. These findings not only clarify the contentious key issue regarding to the amplification mechanism of N 2 + lasing but also show the unique characteristics of ultrashort laser-induced amplification in a molecular ion system where both the microscopic and macroscopic quantum coherence might be present.
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.