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Journal of the Physical Society of Japan

Three-Level Maser Action in Gas II. Experimental Study on Formic Acid

Tatsuo Yajima

Published Sep 1, 1961• 11 citations
Publisher

Abstract

The quantum mechanical behavior of the three-level maser was experimentally studied using the rotational spectrum of HCOOH molecule at microwave frequencies. By using the 2 11 ←1 10 line at the frequency of 46581 Mc as the pumping, the induced emission of the 2 11 →2 12 line at the frequency of 4916 Mc was obtained. For a strong pumping, the splitting of emission line due to resonant modulation effect was observed. The line-shape of emission signal under off-resonant pumping was studied in detail. The emission spectrum due to simultaneous emission and absorption of two photons corresponding to the signal and the pumping was observed for the condition of far off-resonant pumping. The results were compared with the theory described in the previous paper, and was found to be in good agreement in many respects. Some discrepancies concerning emission intensity are also discussed. An application of the multiple quantum transition to a four-level system of HC·OOH is described.

DOI
10.1143/jpsj.16.1709

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Physical Review•Sep 15, 1957•258 citations
The quantum mechanical behavior of the three-level maser was experimentally studied using the rotational spectrum of HCOOH molecule at microwave frequencies. By using the 2 11 ←1 10 line at the frequency of 46581 Mc as the pumping, the induced emission of the 2 11 →2 12 line at the frequency of 4916 Mc was obtained. For a strong pumping, the splitting of emission line due to resonant modulation effect was observed. The line-shape of emission signal under off-resonant pumping was studied in detail. The emission spectrum due to simultaneous emission and absorption of two photons corresponding to the signal and the pumping was observed for the condition of far off-resonant pumping. The results were compared with the theory described in the previous paper, and was found to be in good agreement in many respects. Some discrepancies concerning emission intensity are also discussed. An application of the multiple quantum transition to a four-level system of HC·OOH is described.
The multiple quantum process in the off-resonant condition of the three-level gas maser is discussed. The intensity of the emission produced by this process is calculated by a perturbation theory and also by a more general treatment which is the application of Javan's theory to the off-resonant case. Some graphical representations of the signal line under off-resonant pumping are given for the purpose of comparison with experiment. The Doppler effect in three-level maser action is analyzed from both semiclassical and quantum mechanical points of view under the presence of collision relaxation. It was shown that in a saturation process between two levels, Doppler effect behaves as to contribute to both line-width and relaxation time for the transition, and that under strong pumping, Doppler effect in pumping transition has a marked influence on both intensity and shape of the signal line through the effect of multiple quantum transition.
An analysis of a three-level system using time-dependent perturbation theory shows that two distinct photon-emission processes take place within such a system when stimulated optical emission occurs: one-and two-photon transitions. The two-photon transition consists of the emission of a stimulated photon followed by the absorption of a coherent pump photon. In three-level systems which possess a narrow pump level, two-photon transitions are dominant at high pump powers while the maser line is split into two lines due to the modulation of the wave function at an angular frequency determined by the rate of pumping. This might lead to the possibility of frequency-modulating the maser line. These results are extended qualitatively to include optical masers which possess broad pump-bands.
A theory is presented of induced Raman emission in a three-level system whose parameters are appropriate for microwave to optical frequencies. Solutions of the time-dependent Schrödinger equation are obtained for arbitrary intensity of the pump and signal radiations, which are assumed to be not too many line-widths off resonance. It is shown how the quantum-mechanical aspects of the problem may be separated from the statistical-mechanical aspects, in contrast to the density matrix techniques. The frequency dependence of the Raman emission on the frequency and intensity of the pumping radiation obtained by this method is presented and compared with the results we have obtained by other methods. The intensity and line shape of the Raman emission when the pump frequency is far off resonance are also obtained. The case of three interacting fields is also considered.
An analysis of a three-level system using time-dependent perturbation theory shows that two distinct photon-emission processes take place within such a system when stimulated optical emission occurs: one-and two-photon transitions. The two-photon transition consists of the emission of a stimulated photon followed by the absorption of a coherent pump photon.In three-level systems which possess a narrow pump level, two-photon transitions are dominant at high pump powers while the maser line is split into two lines due to the modulation of the wave function at an angular frequency determined by the rate of pumping. This might lead to the possibility of frequency-modulating the maser line. These results are extended qualitatively to include optical masers which possess broad pump-bands.
An analysis of a three-level system using time-dependent perturbation theory shows that two distinct photon-emission processes take place within such a system when stimulated optical emission occurs: one-and two-photon transitions. The two-photon transition consists of the emission of a stimulated photon followed by the absorption of a coherent pump photon. In three-level systems which possess a narrow pump level, two-photon transitions are dominant at high pump powers while the maser line is split into two lines due to the modulation of the wave function at an angular frequency determined by the rate of pumping. This might lead to the possibility of frequency-modulating the maser line. These results are extended qualitatively to include optical masers which possess broad pump-bands.
In a three-level maser, a transition between two energy levels is saturated in order to produce an induced emission of power at a lower frequency corresponding to a transition between an intermediate energy level and one or the other of the two saturated levels. In this paper, certain effects are discussed which cannot be predicted from a theory in which the population differences alone are considered in this process. For instance, it is shown that, in some cases it is possible to obtain for the same system an induced emission of power at two frequencies given by the resonances between the intermediate energy level and both of the saturated levels. Also, it is shown that, even in the absence of inhomogeneous broadening of the spectral line, one can obtain a net induced emission at some portions of a resonant line and a net absorption at other frequencies within the line widths. Such effects become important even in early stages of saturation in cases where T1=T2{T}_{1}={T}_{2}T1​=T2​ which is true for ordinary gaseous systems and individual spin systems in a majority of very dilute paramagnetic solids. A complete theory is discussed for a gaseous system and extended to two limiting cases of paramagnetic materials with T1=T2{T}_{1}={T}_{2}T1​=T2​ and ${T}_{2}\ensuremath{\ll}{T}_{1}$ for each individual spin system. Furthermore, it is shown that for a saturating field of fixed frequency, the integral of induced power over the entire line is in full agreement with the results of a semiclassical treatment in which the population differences alone are considered. Some remarks are made as to the practicability of certain systems of this type.