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Physical Review A

Vibrational and electronic excitation of ionized nitrogen molecules in intense laser fields

Xunqi Zhong, Zhiming Miao, Linlin Zhang, Qingqing Liang, Mingwei Lei, Hongbing Jiang, Yunquan Liu, Qihuang Gong, Chengyin Wu

Published Oct 26, 2017• 42 citations
Publisher

Abstract

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.

DOI
10.1103/physreva.96.043422

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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.
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.
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.
Nitrogen molecules in ambient air exposed to an intense near-infrared femtosecond laser pulse give rise to cavity-free superradiant emission at 391.4 and 427.8 nm. An unexpected pulse duration-dependent cyclic variation of the superradiance intensity is observed when the central wavelength of the femtosecond pump laser pulse is finely tuned between 780 and 820 nm, and no signal occurs at the resonant wavelength of 782.8 nm (2ω_{782.8 nm}=ω_{391.4 nm}). On the basis of a semiclassical recollision model, we show that an interference of dipolar moments of excited ions created by electron recollisions explains this behavior.
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.