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IEEE Journal of Quantum Electronics

Influence of vibrational, rotational, and reorientation relaxation on pulse amplification in molecular amplifiers

F. A. Hopf, C. K. Rhodes

Published Jun 1, 1972• 0 citations
Publisher
DOI
10.1109/jqe.1972.1077141

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Influence of Vibrational, Rotational, and Reorientational Relaxation on Pulse Amplification in Molecular Amplifiers

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Short-pulse amplification in gaseous molecular amplifiers is complicated by many aspects of atomic and molecular interactions. Among these are the various vibrational, rotational, and reorientational relaxational processes which influence the coupling of the energy stored in the molecular radiators to the electromagnetic field. The properties of plane-wave pulse amplification, especially in the saturated regime, are examined numerically in order to quantitatively determine the detailed effects of these relaxational phenomena. As expected, the results for saturated amplification show that the amount of extracted energy decreases significantly when the rotational relaxation time is sufficiently long in comparison to the pulse width. We also observe the development of pulse-shape variations which are a direct result of the collisional phenomena and differ qualitatively from the results obtained for amplifying media without an energy reservior. There is a tendency for the pulse lengths to increase owing to the energy transfer, in contrast to the strong narrowing effects which occur in the absence of the collisional processes. The influence of reorientational collisions is found to be small, accounting for less than a 20% effect on the over-all conclusions. Finally, we present results concerning the development of an asymptotic pulse shape in high-gain amplifiers. In this case, the pulse shape clearly exhibits the competition between the stimulated rate, which scales with the optical flux, and the collisional rates which are determined by the particle density. Calculations of this nature may be applied directly to C${\mathrm{O}}_{2}$, CO, and HF molecular amplifiers for both the electrically and chemically driven systems.

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Probing the quantum noise level with respect to a coherent input has recently received much attention. Several researchers have probed this question by examining the level of external optical input needed to influence the output field of a quantum noise amplifier. For example, it has been found that it takes, on average, about one photon per (temporal) mode to control the phase of the output field of a Raman amplifier.1 A similar result has been seen in optical parametric amplification.2 In contrast to using light to seed the amplification, we have investigated the level of initial molecular coherence needed to control the phase of the output field of a Raman amplifier. Two laser pulses, separated in time, were used to pump a common set of hydrogen molecules producing two Stokes pulses via stimulated Raman scattering. The relative phase of the two Stokes pulses was measured interferometrically. The variance of this relative phase is a direct measure of the memory of the molecular coherence that was induced by the first scattering process. Correlations between the two Stokes phases were observed even after nine molecular dephasing times, when the level of coherence had decayed by a factor of e−9. We show that this extraordinarily long-lived phase memory comes about because a molecular coherence corresponding to order ten vibrational photons per mode is sufficient to influence the phase of the output field.

Annual Meeting Optical Society of America•Jan 1, 1991•0 citations
Short-pulse amplification in gaseous molecular amplifiers is complicated by many aspects of atomic and molecular interactions. Among these are the various vibrational, rotational, and reorientational relaxational processes which influence the coupling of the energy stored in the molecular radiators to the electromagnetic field. The properties of plane-wave pulse amplification, especially in the saturated regime, are examined numerically in order to quantitatively determine the detailed effects of these relaxational phenomena. As expected, the results for saturated amplification show that the amount of extracted energy decreases significantly when the rotational relaxation time is sufficiently long in comparison to the pulse width. We also observe the development of pulse-shape variations which are a direct result of the collisional phenomena and differ qualitatively from the results obtained for amplifying media without an energy reservior. There is a tendency for the pulse lengths to increase owing to the energy transfer, in contrast to the strong narrowing effects which occur in the absence of the collisional processes. The influence of reorientational collisions is found to be small, accounting for less than a 20% effect on the over-all conclusions. Finally, we present results concerning the development of an asymptotic pulse shape in high-gain amplifiers. In this case, the pulse shape clearly exhibits the competition between the stimulated rate, which scales with the optical flux, and the collisional rates which are determined by the particle density. Calculations of this nature may be applied directly to CO2{\mathrm{O}}_{2}O2​, CO, and HF molecular amplifiers for both the electrically and chemically driven systems.
Probing the quantum noise level with respect to a coherent input has recently received much attention. Several researchers have probed this question by examining the level of external optical input needed to influence the output field of a quantum noise amplifier. For example, it has been found that it takes, on average, about one photon per (temporal) mode to control the phase of the output field of a Raman amplifier.1 A similar result has been seen in optical parametric amplification.2 In contrast to using light to seed the amplification, we have investigated the level of initial molecular coherence needed to control the phase of the output field of a Raman amplifier. Two laser pulses, separated in time, were used to pump a common set of hydrogen molecules producing two Stokes pulses via stimulated Raman scattering. The relative phase of the two Stokes pulses was measured interferometrically. The variance of this relative phase is a direct measure of the memory of the molecular coherence that was induced by the first scattering process. Correlations between the two Stokes phases were observed even after nine molecular dephasing times, when the level of coherence had decayed by a factor of e−9. We show that this extraordinarily long-lived phase memory comes about because a molecular coherence corresponding to order ten vibrational photons per mode is sufficient to influence the phase of the output field.