Argon gas excited by resonant femtosecond ultraviolet pulses gives rise to cavity-free lasing emission in the near-infrared (NIR) range. Here we reported on a pump-probe study of the optical gain of this lasing phenomenon. With the injection of an external seeding pulse, the forward signal was significantly enhanced, confirming the existence of optical gain. The temporal dynamics of the optical gain were characterized by a time-resolved measurement. It was found that the optical gain decays on a time scale of ∼ 10 ps and it does not present a significant dependence on the gas pressures. Moreover, the intensity of the forward NIR emission signal shows a linear dependence on the gas pressure. These features suggest that the nature of this forward NIR radiation is amplified spontaneous emission, not superradiance when multiple-photon resonant excitation is involved.
Argon gas excited by resonant femtosecond ultraviolet pulses gives rise to cavity-free lasing emission in the near-infrared (NIR) range. Here we reported on a pump-probe study of the optical gain of this lasing phenomenon. With the injection of an external seeding pulse, the forward signal was significantly enhanced, confirming the existence of optical gain. The temporal dynamics of the optical gain were characterized by a time-resolved measurement. It was found that the optical gain decays on a time scale of ∼ 10 ps and it does not present a significant dependence on the gas pressures. Moreover, the intensity of the forward NIR emission signal shows a linear dependence on the gas pressure. These features suggest that the nature of this forward NIR radiation is amplified spontaneous emission, not superradiance when multiple-photon resonant excitation is involved.
Nitrogen ions pumped by intense femtosecond laser pulses present an optical gain at 391.4 nm, evident by energy amplification of an injected resonant seeding pulse. We report a time-resolved measurement of the amplification process with seeding pulses having varying intensities. It is found that the amplification factor depends on the intensity of the seeding pulse and the effective temporal window for the optical gain becomes longer by applying more intense seeding pulses. These two features are in sharp contrast with classic pump-probe experiments, pinpointing the crucial role of macroscopic coherence and its dynamics during the lasing process. We further measure the temporal profile of the amplified emission for seeding pulse injected at different time delays. A complicated temporal behavior is observed, which highlights the nature of the superfluorescence.
We investigate the dynamics of cavity-free lasing from neutral nitrogen molecules in femtosecond laser filaments. An important difference of intensity and temporal duration is observed between backward and forward lasing, in both amplified spontaneous emission and seed-amplification regimes. Numerical simulations based on a nonadiabatic Maxwell-Bloch model reproduce well the observations, and attribute these differences to the finite gain lifetime and the traveling excitation nature of this gas laser.
Multiple gain routes complicate the amplification behaviors of N2+ lasing. A direct comparison of the amplification processes of various lasing lines of N2+ is still lacking to date, mainly because the efficient generation of different lasing lines requires different experimental conditions. In this work, to overcome the limitation, we use an intense polarization-modulated femtosecond laser pulse to simultaneously produce high-intensity N2+ lasing signals at 391 nm and 428 nm, permitting us readily performing their time-domain characterizations. Our results show that the primary amplification of 428-nm lasing is always retarded by a few picoseconds with respect to the probe pulse while the amplification of 391-nm lasing can be basically completed within the probe pulse duration at a relatively high gas pressure, and besides, the time duration of the former sustains several times longer than that of the latter. These observations indicate the non-negligible contribution of the initial electronic coherence established by the pump laser, apart from the external triggering pulse. For the 391-nm lasing, the seed amplification and superradiance can fiercely interplay within the probe pulse duration. However, for the 428-nm lasing, its amplification is in essence Raman-assisted superfluorescence due to the lacking of the initial electronic coherence and a direct triggering pulse. Our findings not only shed light on the physics of N2+ lasing but also promote the relevant studies on the collective emissions in the cascaded multi-level molecular ion system.
Coherent control of the multiple wavelength lasing of 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.
There exists a lack of laser-based remote sensing methods that give signals with high intensity and directionality. According to previous research, mirrorless lasing can meet these requirements; however, neither the dependence on the gain medium geometry nor the light-matter interaction responsible for the emission has been investigated in detail. This thesis project examined the sideways lasing emission from a gain medium with a Fresnel number much smaller than one, generated by the overlap of two counterpropagating femtosecond laser pulses in xenon gas at atmospheric pressure. Both spatial and temporal measurements of the sideways lasing emission were made, with the latter being obtained using a streak camera. The emission was highly localised in space, suggesting it originated from the overlap. It also yielded a power dependence with a clear threshold and an interference pattern indicating coherence, both of which showed strong agreement with the predicted behaviour for superfluorescence (SF). The recorded temporal profile displayed a pulse with oscillations on the incline and the decline, appearing with a delay of about 70 ps relative to the excitation pulse and thus corresponding well to the theoretical predictions for SF emitted from a gain medium with a Fresnel number much smaller than one. It can therefore be concluded that the observed sideways lasing was generated by SF. Additionally, the dependence of the emission on the gain medium geometry was in good accordance with theory. These measurements, to the best of the author's knowledge, provide the first thorough investigation of mirrorless lasing at atmospheric pressure for this gain medium configuration, thus opening the way for both further fundamental research and the implementation of these techniques in applied laser diagnostics.
Air lasing induced by laser filamentation opens a new route for research on atmospheric molecular physics and remote sensing. The generation of air lasing is composed of two processes, i.e., building up optical gain of air molecules in femtosecond time scale and emitting coherent radiation in picosecond time scale. Here, we focus on the emission mechanisms of N 2 + air lasing and reveal, by examining the intensities and temporal profiles of N 2 + lasing at 391 nm generated respectively in a time-varying polarization-modulated and a linearly polarized pump laser field under different nitrogen gas pressures, that the N 2 + lasing can emit through either triggered super-radiance or seed amplification. We find that the two pressure-sensitive factors, i.e., the dipole dephasing time T 2 and the population inversion density n , determine which of these two mechanisms dominates the N 2 + lasing emission process, enabling manipulation of the transition from triggered super-radiance to seed amplification or vice versa. Our findings clarify the emission mechanism of N 2 + lasing under different pressures and provide a deeper understanding of N 2 + air lasing not only in the establishment of optical gain but also in the lasing emission process.