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Journal of the Optical Society of America B

Photon echoes using double-resonance optical pulses

Ning Lü, P. R. Berman

Published Dec 1, 1985• 3 citations
Publisher

Abstract

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.

DOI
10.1364/josab.2.001883

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Physical Review A•Nov 1, 1979•164 citations
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.
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.
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.
The coherent excitation of a three level atom by one- and two-photon resonances coupled by a common level is treated by the method of averages. The equations for the density matrix of the three resonant levels are solved analytically for square pulses of duration shorter than relaxation times. Double free induction decay occuring when both exciting fields are switched out of resonance simultaneously is exhibited. The emitted radiation is also calculated for an experiment in which the field driving the one-photon resonance remains on after the other field ends, and it is shown that experiments at several detunings and amplitudes would allow determination of various combinations of relaxation rates. Numerical studies for nonsquare pulses are briefly described. The results show that the main qualitative features of the square-pulse case are retained. 15 references.
The possible generation of photon echoes is discussed for a system where the incident radiation resonantly drives two-photon transitions. Use of the adiabatic-vector-model approximation of Grischkowsky, Loy, and Liao allows echo behavior to be calculated in a multilevel system by methods similar to those previously employed for two-level atoms. We find that observation of the double-quantum photon echo requires the presence of a nonresonant probe field at the time of formation of the echo pulse. The echo then radiates at the sum and difference of the probe and two-photon frequencies. As an example, we consider a possible experimental arrangement for the detection of double-quantum photon echoes in Rb vapor.
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 primary objective of this paper is to provide a formalism to predict and characterize the echoes which may be produced in a gaseous sample by an arbitrary sequence of one- or two-frequency laser excitation pulses which successively transfer atomic population between two or more atomic energy levels. The resulting echoes can occur at times which depend on the relative frequencies of the excitation pulses as well as on the times at which the pulses were applied. Using an idealized model of the excitation pulses and the atoms, the authors derive a simple transformation equation which provides the density matrix of a single atom after a general excitation sequence. Equations are derived which utilize the single-atom density matrix to predict the properties of the echoes (if any) which result. The means by which the sample of atoms "remembers" the information necessary to produce different types of echoes is discussed, and it is then shown how a study of the echo can provide information concerning the atomic relaxation processes which tend to destroy this information. It is observed that trilevel echoes can be used to determine the relaxation characteristics of superposition states between energy levels coupled by two-photon transitions. In the case of certain other echoes (such as the three-excitation-pulse stimulated echo) the authors discuss the heretofore unappreciated fact that the sample remembers the "echo information" via a nonthermal velocity distribution of the atoms in one specific atomic state. In these cases a study of the echo behavior can provide information pertaining to the relaxation processes affecting only the one atomic state. The formalism developed is used to predict the properties of several echo effects. First, to provide a connection with previous work, the well-known photon echo is briefly discussed. Then important new properties of the three-excitation-pulse-stimulated echo are described. Finally, three different types of trilevel echo are analyzed. Each of the trilevel echoes discussed has widespread applicability in the study of relaxation processes.