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Applied Physics Letters

Femtosecond pump-probe studies of atomic hydrogen superfluorescence in flames

Kai Wang, Yejun Wang, Jizhou Wang, Zhenhuan Yi, Waruna D. Kulatilaka, Alexei V. Sokolov, Marlan O. Scully

Published May 18, 2020• 6 citations
Publisher

Abstract

We investigate the excited-state dynamics of hydrogen (H) atoms in flames by using a femtosecond (fs) pump-probe scheme and measuring directional emission signals. An approximately 100-fs pump pulse at 205.1 nm excites H atoms through a two-photon process (n = 3 ←← n = 1), which is followed by detection of the forward emission signals induced by a broadband fs probe pulse near 656 nm. Above a certain threshold, we observe a quadratic dependence of the emission signal on the pump laser energy. Moreover, the linewidth of the forward emission signal varies with the probe delay and the probe laser energy. This behavior can be explained in terms of superradiance. We perform a theoretical analysis and compare the experimental results with the theory, and conclude that, within the conditions of our experiment, the behavior of the atomic system involves atomic coherence, which is produced non-adiabatically and corresponds to a superradiant process. Variations in the duration of the gain time window and lifetime of the excited-state H atoms in flames are explored at different flame conditions (i.e., equivalence ratio and heights above the burner). The fs pump-probe technique demonstrated here can also be extended to characterize the time-resolved population dynamics and the corresponding collisional energy transfer rates for energy levels involved in laser-induced fluorescence detection of H atoms in flames relevant to practical combustion applications.

DOI
10.1063/5.0001924

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We investigate the excited-state dynamics of hydrogen (H) atoms in flames by using a femtosecond (fs) pump-probe scheme and measuring directional emission signals. An approximately 100-fs pump pulse at 205.1 nm excites H atoms through a two-photon process (n = 3 ←← n = 1), which is followed by detection of the forward emission signals induced by a broadband fs probe pulse near 656 nm. Above a certain threshold, we observe a quadratic dependence of the emission signal on the pump laser energy. Moreover, the linewidth of the forward emission signal varies with the probe delay and the probe laser energy. This behavior can be explained in terms of superradiance. We perform a theoretical analysis and compare the experimental results with the theory, and conclude that, within the conditions of our experiment, the behavior of the atomic system involves atomic coherence, which is produced non-adiabatically and corresponds to a superradiant process. Variations in the duration of the gain time window and lifetime of the excited-state H atoms in flames are explored at different flame conditions (i.e., equivalence ratio and heights above the burner). The fs pump-probe technique demonstrated here can also be extended to characterize the time-resolved population dynamics and the corresponding collisional energy transfer rates for energy levels involved in laser-induced fluorescence detection of H atoms in flames relevant to practical combustion applications.
Lasing refers to the generation of highly directional laser-like emission remotely pumped by laser pulses in a medium such as ambient air or a flame.It has been intensively investigated because of its potentials to revolutionize the field of remote sensing.Earlier studies were carried out in flames, where lasing effect has been observed in various radicals, for example H, O, N etc., through two-photon resonant excitation.This scheme was later applied to generate lasing of O and N in ambient air, which can be dramatically improved by predissociation of the air constituents.However, the underlying physical mechanism of two-photon-excited lasing effect is still unsettled although it has been studied for more than one decade.Currently there are three different proposals: (1) Amplified Spontaneous Emission (ASE), in which case population inversion is responsible for optical gain;(2) Superfluorescence (SF), where a macroscopic dipole occurs in the population inverted medium; (3) Both hyper-Raman scattering and four-wave mixing are involved in the generation of lasing emission.Here, we experimentally studied 656 nm lasing emission of atomic hydrogen via two-photon resonant excitation by focusing 125-fs laser pulses of 205-nm wavelength in a methane/oxygen welding flame (see Fig. 1), where hydrogen atoms are naturally present.Lasing occurs in both forward and backward directions, and the forward signal strength is almost one order of magnitude stronger than the backward one.It has been found that the durations of lasing pulses are around 20 ps, and decreases with increasing pump laser energies.Furthermore, the delay of the lasing pulse with respect to the pump pulse decreases with increasing pump energies.These results show high similarities with the behaviors of SF, suggesting that the femtosecond two-photonexcited lasing emission of atomic hydrogen might be SF.
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We study the superfluorescence (SF) from a gas of rubidium atoms. The atoms of a dense vapor are excited to the 5D5D5D state from the 5S5S5S state by a two-photon process driven by 100-fs laser pulses. The atoms decay to the 6P6P6P state and then to the 5S5S5S state. The SF emission at 420 nm on the 6P6P6P--5S5S5S transition is recorded by a streak camera with picosecond time resolution. The time duration of the generated SF is tens of picoseconds, which is much shorter than the time scale of the usual relaxation processes, including spontaneous emission and atomic coherence dephasing. The dependence of the time delay between the reference input pulse and SF is measured as a function of laser power. The experimental data are described quantitatively by a simulation based on the semiclassical atom-field interaction theory. The observed change in scaling laws for the peak intensity and delay time can be elucidated by an SF theory in which the sample length is larger than the cooperation length.
Strong excitation with high electromagnetic fields can generate lasing in gaseous media by resonant excitation. Previous efforts have shown that the lasing signal can be emitted perpendicular to the direction of the pump laser if the shape of the gain volume can be controlled. This paper reports on the characterization of sideways emitted lasing obtained through two-photon pumping in oxygen atoms present in a flame. Intense 35-fs laser pulses of 226-nm wavelength focused into a sheet by a cylindrical mirror are used to form a gain volume geometry that yields an 845-nm lasing beam that is emitted perpendicular to the pump-beam direction. The sideways lasing has been investigated in terms of its pump laser energy dependence, excitation and emission spectra, and spatial characteristics. Single-shot images of the emission exhibit interference fringes, revealing that the emission contains multiple coherent spatial modes. The results indicate that superfluorescence constitutes a significant contribution to the sideways lasing. We believe that this is the first important step for understanding and using sideways lasing as a phenomenon and tool for future applications and inventions.