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Optics Express

Vibrational Raman scattering from coherently excited molecular ions in a strong laser field

Bo Xu, Jinping Yao, Yuexin Wan, Jinming Chen, Zhaoxiang Liu, Fangbo Zhang, Wei Chu, Ya Cheng

Published Jun 14, 2019• 11 citations
Publisher

Abstract

We report on a pump-probe investigation of vibrational Raman scattering from coherently excited N2+ ions. It is found that the Raman signals produced by the inelastic scattering of the probe pulse from molecular ions can be dramatically enhanced when the probe laser is resonant with electronic transitions in N2+ ions. The Raman signal can be amplified at 428 nm wavelength due to the presence of population inversion in N2+ ions.

DOI
10.1364/oe.27.018262

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We report on a pump-probe investigation of vibrational Raman scattering from coherently excited N2+ ions. It is found that the Raman signals produced by the inelastic scattering of the probe pulse from molecular ions can be dramatically enhanced when the probe laser is resonant with electronic transitions in N2+ ions. The Raman signal can be amplified at 428 nm wavelength due to the presence of population inversion in N2+ ions.
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We report a combined theoretical and experimental investigation on the unambiguous role of electronic coherence underlying the generation of laserlike coherent emission from N2+{{\mathrm{N}}_{2}}^{+}N2​+ ions launched in a strong laser field. The coherence manifests itself by giving rise to a dramatic enhancement of N2+{{\mathrm{N}}_{2}}^{+}N2​+ laserlike radiation with two temporally separated pump laser pulses centered at 800- and 1580-nm wavelengths, respectively. We further show that coherent control of N2+{{\mathrm{N}}_{2}}^{+}N2​+ lasing in a subfemtosecond timescale can be achieved by replacing the single 800-nm laser pulse with a pair of 800-nm laser pulses of adjustable time delay. The experimental results are well reproduced in theory using a three-level quantum model of N2+{{\mathrm{N}}_{2}}^{+}N2​+ ions under the density matrix representation.
We report on the generation of cascaded rotational Raman scattering up to 58th order in coherently excited CO2\mathrm{C}{\mathrm{O}}_{2}CO2​ molecules. Raman scattering with more than 600 sidebands is obtained using an intense femtosecond laser to impulsively excite rotational coherence and femtosecond-laser-induced N2+{{\mathrm{N}}_{2}}^{+}N2​+ lasing to generate cascaded Raman signals. This configuration allows this experiment to be performed with a single femtosecond laser beam at free-space standoff locations. It is revealed that the efficient spectral extension of Raman signals is attributed to the specific structures of N2+{{\mathrm{N}}_{2}}^{+}N2​+ lasing in the spectral and temporal domains and the ideal spatial overlap of the femtosecond laser and N2+{{\mathrm{N}}_{2}}^{+}N2​+ lasing. A Raman spectrum extending above $2000\phantom{\rule{0.16em}{0ex}}\mathrm{c}{\mathrm{m}}^{\ensuremath{-}1}$ naturally corresponds to a femtosecond pulse train due to the periodic revivals of molecular rotational wave packets.
We have considered the Raman scattering in molecular media. Applying two laser fields in a two-photon resonance with vibrational transition, we have studied the role of rotational levels for excitation of vibrational coherence. It is shown that the molecular vibrational coherence strongly depends on the effect of coherent population trapping for rotational levels. The obtained results are important for applications of Raman spectroscopy to molecular detection in engineering, chemical, and biological applications.
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 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.