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Physical Review A

Ionization-coherence-enhanced-vibration photoexcitation in nitrogen ions

Chaohui Zhou, Liang Xu, Jiahao Dong, Sheng Li, Yuanqian Yang, Zhengyang Bai, Feng He, Aurélien Houard, A. Mysyrowicz, Vladimir T Tikhonchuk, Yi Liu

Published May 23, 2025• 2 citations
Publisher

Abstract

We develop a vibronic coherence model for multiorbital ionization and excitation of nitrogen molecules, based on an up-to-date concept of coherent ionization into excited states [C. H. Yuen and C. D. Lin, Phys. Rev. A 108, 023123 (2023); Phys. Rev. A 109, 033108 (2024)]. Compared to other models, where the coherence of excitation dynamics is described with fewer details, our model predicts larger populations at excited states, in particular, at levels corresponding to the transition wavelengths 391 or 428 nm relevant to air lasing in the atmospheric environment. The dependence of population inversion on the pump wavelength is investigated, showing that ionic coherence in ionization injection enhances the vibronic three-photon transition in the ${\mathrm{N}}_{2}$ postionization process.

DOI
10.1103/physreva.111.053117

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We develop a vibronic coherence model for multiorbital ionization and excitation of nitrogen molecules, based on an up-to-date concept of coherent ionization into excited states [C. H. Yuen and C. D. Lin, Phys. Rev. A 108, 023123 (2023); Phys. Rev. A 109, 033108 (2024)]. Compared to other models, where the coherence of excitation dynamics is described with fewer details, our model predicts larger populations at excited states, in particular, at levels corresponding to the transition wavelengths 391 or 428 nm relevant to air lasing in the atmospheric environment. The dependence of population inversion on the pump wavelength is investigated, showing that ionic coherence in ionization injection enhances the vibronic three-photon transition in the N2{\mathrm{N}}_{2}N2​ postionization process.
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 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.
Tunneling ionization, a fascinating quantum phenomenon, has played the key role in the development of attosecond physics. Upon absorption of a few tens of photons, tunneling ionization creates ions in different excited states and even enables the formation of population inversion between ionic states. However, the underlying physics is still being debated. Here, we demonstrate a significant enhancement in the efficiency of multiphoton excitation when ionization of neutral molecules and resonant excitation of ions coexist in strong laser fields. It facilitates the dramatic increase in population inversion and lasing radiation in N_{2}^{+} around 1000 nm pump wavelength. Utilizing the ionization-coupling theory, we discover that the synergistic interplay between tunneling ionization and multiphoton excitation enables the ionic coherence to be maximized by phase locking of the periodically created ionic dipoles and consistently maintain an optimal phase for the follow-up photoexcitation. This Letter provides new insights into the photoexcitation mechanism of ions in strong laser fields and opens up a route for optimizing ionic lasing radiations.
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.
The existence of electronic coherence can fundamentally change the scenario of nonlinear interaction of light with quantum systems such as atoms and molecules, which, however, has escaped from observation in the investigations of strong field nonlinear optics in the past several decades. Here, we report on the generation of electronic quantum coherence by strong field ionization of nitrogen molecules in an intense 800 nm laser field. The coherence is experimentally revealed by observing a resonant four-wave mixing process in which the two pump pulses centered at 800 nm and 1580 nm wavelengths are temporally separated from each other. The experimental observation is further reproduced by calculating the nonlinear polarization response of N_2^+ ions using a three-level quantum model. Our result suggests that strong field ionization provides a unique approach to generating a fully coherent molecular wavepacket encapsulating the rotational, vibrational, and electronic states.
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.