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Register a new userNear-resonant Raman amplification in the rotational quantum wavepackets of nitrogen molecular ions generated by strong field ionization
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Generation of laser-like narrow bandwidth emissions from nitrogen molecular ions generated in intense near- and mid-infrared femtosecond laser fields has aroused much interest because of the mysterious physics underlying such a phenomenon as well as the potential application of such an effect in atmospheric spectroscopic sensing. Here, we perform a pump-probe measurement on the nonlinear interaction of rotational quantum wavepackets of nitrogen molecular ions generated in mid-infrared (e.g., at a wavelength centered at 1580 nm) femtosecond laser fields with an ultrashort probe pulse whose broad spectrum overlaps both P- and R-branch rotational transition lines between the upper and lower electronic states. The results show that in the near-resonant conditions, stimulated Raman amplification can efficiently occur which converts the broad bandwidth ultrashort probe pulse into the narrow bandwidth laser-like beam. Our finding provides an insight into the physical mechanism of strong field induced lasing actions in atmospheric environment.
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Generation of free-space laser-like emissions of high spatiotemporal coherence and narrow bandwidth in atmosphere opens promising opportunities for remote spectroscopic sensing. Here, we report on generation of such laser-like emissions, which results from the combined contributions of perturbative and non-perturbative nonlinear optical effects in nitrogen molecules exposed to intense mid-infrared laser fields. We systematically investigate the dependence of the generated free-space laser spectrum on wavelength and power of the driver laser. It is revealed that the free-space laser is produced by resonant Raman amplification of the fifth harmonic of the driver pulses in rotational wavepacket of the molecular nitrogen ions.
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 perform a combined theoretical and experimental investigation of the superradiance in the quantum coherent system generated by strong laser fields. The semiclassical theory of superradiance that includes the superradiant temporal profile, character duration, time delay, intensity is derived. The experimental data and theoretical predictions of 391-nm forward emission as a function of nitrogen gas pressure are compared and show good agreement. Our results not only demonstrate that the time-delayed optical amplification inside the molecular nitrogen ions is superradiance, but also reveal the quantum optical properties of strong-field physics.
A new mode of effective interaction of molecular rotational degrees of freedom with an intense, nonresonant, ultrashort laser pulse is explored. Transient nonadiabatic charge redistribution (TNCR) in larger molecules or molecular ions causes impulsive-torque interaction that replaces the traditional mechanism of molecular alignment based on perturbative interaction of the laser field with electronic subsystem as manifested in linear anisotropic polarizability or hyperpolarizability. We explore this new alignment mechanism on a popular generic model of a tight-binding diatomic molecule. We consider the case of rotational wavepacket formation when a molecule is initially in the ground rotational state. The rotational wavepacket emerging from the TNCR interaction consists of states with higher rotational quantum numbers, in comparison with the anisotropic-polarizability case, and the after-pulse alignment oscillations are out-of-phase with those resulting from the traditional interaction. The TNCR interaction mode is expected to play a major role when a strong laser field actually causes extensive nonresonant excitation and/or ionization of a molecule.
We demonstrate a route to supercontinuum generation in gas-filled hollow-core anti-resonant fibers through the creation of a broad vibrational Raman frequency comb followed by continuous broadening and merging of the comb lines through either rotational Raman scattering or the optical Kerr effect. Our demonstration experiments, utilizing a single pump pulse with 20 ps duration at 532 nm in a nitrogen-filled fiber, produce a supercontinuum spanning from 440 nm to 1200 nm, with an additional deep ultraviolet continuum from 250 nm to 360 nm. Numerical results suggest that this approach can produce even broader supercontinuum spectra extending from the ultraviolet to mid-infrared.
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