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Journal of Experimental and Theoretical Physics

Polarization features of coherent transition phenomena in two-photon resonance

Ashat M. Basharov, V. I. Malmistov, Edward A. Manykin

Published Feb 1, 1983• 0 citations
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Resonance Frequency Shift in Two-Photon Transitions

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A theory of photon echoes using double-resonance optical pulses (PEDROP) is presented. Two double-resonance pulses, separated by a time interval T, are used to cause transitions among three states of an atom. Each double-resonance pulse consists of two simultaneously applied laser pulses that drive coupled transitions in the atom. It is shown that for time t > T, six photon echoes are produced (three on each of the coupled transitions) at five distinct times. Moreover, a nonradiating macroscopic coherence is also produced between states of the same parity. With the use of an interrogation pulse to monitor this coherence, three additional photon echoes can be produced on either of the coupled transitions. A Doppler phase diagram is constructed that enables one easily to predict the times and conditions of echo formation. PEDROP combines features of both two-photon and trilevel echoes but offers advantages over these methods for studying relaxation phenomena.
The degree of linear polarization P L for two-photon absorption of alkali atoms in intermediate strength magnetic fields has been computationally investigated. Polarization spectra were obtained for n a s 2 S 1/2 to n b s 2 S 1/2 transitions with the photons in near resonance with intermediate 2 P j levels. Previous experiments and calculations in the absence of a magnetic held revealed a complete polarization reversal (P L approximately -100%) for frequencies near resonance between the 2 P 1/2 and 2 P 3/2 levels due to fine-structure coherence. Application of weak to intermediate strength fields induce additional depolarization features as a result of anomalous Zeeman splitting. The fine-structure depolarization feature disappears for strong fields (Paschen-Back regime), while the calculations predict that Zeeman depolarization persists though the transitions become forbidden. Magnetic-field-dependent polarization spectra can be measured in the laboratory with high precision and it should prove interesting to trace through the weak, intermediate, and strong field regimes.
Coherent transient phenomena can be generated by the abrupt changes of parameters either of the electromagnetic field or of the matter. Comparative analysis of these two approaches, made on the base of experimental research in molecular gases SF6, 15NH3, HFCO and 13CH3F, excited by the radiation of CW CO2 and 13CO2 lasers, is presented. The first approach of photon echo (and its modifications) generation, based on electro-optic pulses formation from the resonant CW exciting radiation, has proven to be successful for intense infrared molecular transitions. The coherent responses are sufficiently powerful to be applied in high resolution spectroscopy, the spectral markers creation ,and molecular collisions investigations. However, this technique is not very effective for the free polarization decay investigations. Another approach based on the Stark switching molecular levels of polar gas, irradiated by CW laser, was demonstrated for free polarization decay and photon echo generation in 13CH3F. Free polarization decay has shown the pronounced frequency shift because of dynamic Stark effect in the CW radiation field. This specific feature of coherent transients, created by Stark switching, limits the high resolution spectroscopy by the low intensity range of exciting radiation. From other viewpoint, it gives unique possibility to investigate coherent transients generated at the dressed molecular levels.