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Journal of Physics A Mathematical Nuclear and General

Theoretical study of photon echoes associated with the coherent nonlinear optical effect in a resonant three-level system

M. Aihara, Humio Inaba

Published Nov 1, 1973• 21 citations
Publisher

Abstract

An analytical study of the photon echoes associated with the three-level system interacting resonantly with optical pulses possessing two different frequencies is performed. It is predicted that photon echoes arise at anomalous times corresponding to the correlation between the inhomogeneous broadenings for the different spectral lines as well as at the normal time expected in a simple two-level system. This new effect is caused by the coupling of the two resonant transitions through the common energy level. Furthermore, if the particle does not have inversion symmetry, the echoes with the sum or difference frequency of the exciting optical pulses can be observed in such a system. The quantitative analysis is also given for intensities, direction of propagation and polarizations of the anomalous echoes which depend upon the exciting pulses with different frequency.

DOI
10.1088/0305-4470/6/11/009

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An analytical study of the photon echoes associated with the three-level system interacting resonantly with optical pulses possessing two different frequencies is performed. It is predicted that photon echoes arise at anomalous times corresponding to the correlation between the inhomogeneous broadenings for the different spectral lines as well as at the normal time expected in a simple two-level system. This new effect is caused by the coupling of the two resonant transitions through the common energy level. Furthermore, if the particle does not have inversion symmetry, the echoes with the sum or difference frequency of the exciting optical pulses can be observed in such a system. The quantitative analysis is also given for intensities, direction of propagation and polarizations of the anomalous echoes which depend upon the exciting pulses with different frequency.
The theoretical analysis on photon echoes is reported in a resonant multi-level system with level degeneracy, by a general consideration. With respect to the system possessing more than three-fold degeneracy, the intensity of photon echoes depends not only on the areas of the exciting optical pulses, but also on their polarization characteristics. In particular, it was found that some anomalous echoes change their intensities with the polarization directions of exciting optical pulses which have different frequencies from those of the echoes because of the coherent coupling of resonant transitions with common energy level and the interference effect of transitions through the degenerate sublevels. In the first half of this paper the general formulation on the multi-level system with arbitrary degeneracy is performed, and in the second half, the application of the general theory to some typical examples is also given.
Photon echoes, observed recently in ruby and in NH2{\mathrm{NH}}_{2}NH2​D gas by two-pulse laser excitation, exhibit a modulation behavior as the pulse delay time is varied. The effect, which arises in a three-level quantum system, is due to the interference of two optically coupled transitions that share a common level. In this article, the three-level echo problem is treated exactly. Wave-function solutions are incorporated that are handled conveniently by a Laplace-transform technique. We, therefore, extend the earlier theory of echo modulation by Lambert et al., by removing their restriction of on-resonance pulse excitation. This procedure allows us to examine the effect of inhomogeneous broadening on echo amplitude explicitly, and we treat the problem by numerical and also by analytical means for the case of a Doppler-broadened gas. Analytic expressions are derived either for a high or a low laser power regime corresponding to excitation of either a large or a small fraction of the Doppler linewidth. The former case is analogous to pulsed nuclear magnetic resonance and is well known, whereas the latter result is new and applies to current photon echo measurements.
The authors develop a theoretical analysis which describes coherent nonlinear resonant effects where two optical pulses of different frequencies undergo two-photon self-induced transparency (two-photon SIT) in an inhomogeneously broadened three-level system. The field (Maxwell) and atomic (Schrodinger; density matrix representation) equations are coupled in a self-consistent manner by virtue of the resultant macroscopic polarizations at the two frequencies. This treatment is accomplished under circumstances where atomic coherence plays a predominant role. The resulting equations yield a new two-photon area theorem which gives first the intensity dependent, two-photon absorption law analogous to Beer's law for the one-photon transition. Secondly, a 2 pi Lorentzian pulse solution is derived which propagates without loss at the modified pulse velocity.
This paper discusses the correlation of inhomogeneous broadening at various frequency transitions in three-level systems and how it affects the intensity of the stimulated-photon-echo response. It is shown that the correlation coefficient of inhomogeneous broadening at two different energy transitions and the response intensity of the stimulated photon echo depends on the random interaction parameter m of an optical electron with the local field, which in turn depends on the unequal-spacing parameter of the spectrum of the system.
A new type of three-level photon echo has been predicted and analytically described. In contrast to the conventional three-level echo, whose formation involves three resonant ultrashort excitation pulses spaced in time, two of which are resonant to different optically allowed and adjacent transitions with different frequencies, the echo predicted arises under the conditions of formation of the conventional two-pulse echo and requires only two pump pulses of the same frequency. A theory is developed for the conditions of experiments on generation of a superradiance pulse at the 3 P 0-3 H 6 transition in impurity praseodymium ions in the LaF3 matrix upon ultrashort coherent excitation of the adjacent optically allowed 3 H 4-3 P 0 transition in praseodymium. It is shown that the superradiance pulse after its deexcitation does not polarize the medium at the 3 P 0-3 H 6 generation transition and completely eliminates polarization at the 3 H 4-3 P 0 excitation transition. However, simultaneously, the superradiance pulse transfers the optical coherence from the excitation transition to the optically forbidden 3 H 6-3 H 4 transition. Thus, the phase memory about the effect of the excitation superradiance pulse is retained in the medium within a time interval that is shorter than the irreversible relaxation time of the optically forbidden transition.