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Slow and Fast Light (SL)

Chirped quantum cascade laser induced transient gain in strongly absorbing molecular gases

GEOFFREY DUXBURY, Nigel Langford, Kenneth G. Hay

Published Jan 1, 2008• 0 citations
Publisher

Abstract

Using a mW power chirped pulse quantum cascade laser propagating in a 60 m pathlength Herriott cell, delayed rapid passage and transient gain signals have been observed in the 8 μm spectrum of acetylene.
DOI
10.1364/sl.2008.jmb27

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Rapid passage signals have been observed in which a delayed switch from absorption to emission is observed as the optical density of acetylene in a long path length cell is increased. The delayed switch results in the generation of a large, narrow, transient gain signal. Using numerical solutions of the Maxwell–Bloch equations we have demonstrated that this effect is due to constructive interference between the incident laser field and the field generated by the response of the gaseous medium. This occurs owing to the minimal collisional damping at the low gas pressures within the gas cell, so that the chirp rate of the laser is faster than the collisional reorientation time of the molecules.
In this Letter, a 10 microm quantum cascade laser operating in the intrapulse mode is used observe rapid passage (RP) effects within a 40 cm single-pass gas cell containing low pressures of NH(3). The laser tuning range allows the rotational states J=2 with K=0, 1, and 2 to be probed. We show that the RP structures change as a function of optical density and that the magnitude of the delay in the switch from absorption to emission as a function of increased gas pressure is dependent upon the initial value of K. These measurements are qualitatively well modeled using the Maxwell-Bloch equations.
Recently, the advances in generation and characterization techniques of ultrashort laser pulses made it practical to prepare precisely defined laser pulses, these open up new possibilities for studying and controlling dynamical processes in femtosecond time scale. Hitherto, frequency-synthesized or chirped laser pulses have been widely applied to high-order harmonic generation (HHG) [3], population transfer [4], multiphoton transitions between Rydberg states [5], ect. Both the interference of two-color pulses and the nontrivial time dependence of chirped pulse laser field may lead to very interesting results. Moreover, recent studies have manifested that chirping can also have much impacts on the laser pulses as it propagates through different medium. For example, the propagation properties of chirped soliton pulses in optical nonlinear Kenmedia were investigated by Desaix et al. [6]. The result indicates that the properties of asymptotically emerging solitons depend not only on the magnitude, but also on the form of the initial chirp. In particular, the splitting of an initial pulse into separating soliton pulse pairs only occurs for certain classes of initial chirp functions. The influence of pulse shape and frequency chirp on stability of optical solitons was studied by Klaus and Shaw [7]. They found that destabilization occurs when eigenvalues of an associated Zakharov-Shabat system, which move along the positive imaginary axis with increasing chirp parameter, either are absorbed into the lower half plane or collide with a nother eigenvalue. Furthermore, the signal and group velocities for chirped pulses propagating through a GaAs cavity were measured by Centini et al. [8]. They showed that the chirp substantially modifies the group velocity of the pulse, but leaves the signal velocity unaltered.
Using a low power, rapid (nsec) pulse-modulated quantum cascade (QC) laser, collective coherent effects in the 5 μm spectrum of nitric oxide have been demonstrated by the observation of sub-Doppler hyperfine splitting and also Autler-Townes splitting of Doppler broadened lines. For nitrous oxide, experiments and model calculations have demonstrated that two main effects occur with pulse-modulated (chirped) quantum cascade lasers: free induction decay signals, and signals induced by rapid passage during the laser chirp. In the open shell molecule, NO, in which both Λ-doubling splitting and hyperfine structure occur, laser field-induced coupling between the hyperfine levels of the two Λ-doublet components can induce a large ac Stark effect. This may be observed as sub-Doppler structure, field-induced splittings, or Autler-Townes splitting of a Doppler broadened line. These represent an extension of the types of behaviour observed in the closed shell molecule nitrous oxide, using the same apparatus, when probed with an 8 μm QC laser.