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Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE

Polarization effects in radiation interaction with multilevel quantum systems

Alexander A. Apolonski, K. A. Nasyrov, Anatolii M. Shalagin

Published Oct 21, 1998• 0 citations
Publisher

Abstract

In recent years interest has significantly quickened in investigation of nonlinear optical and spectroscopic phenomena in such unique objects as Rydberg atoms (the atoms in the energy states near the ionization limit) and van der Waals complexes (dimers). These objects are characterized, in particular, by that their energy states are strongly degenerate due to a large value of angular (rotational) momentum. Here, the problem arises of adequate theoretical description of experimental results, especially when polarization peculiarities of nonlinear radiation processes are considered. The problem is caused by the existence of a huge number of quantum magnetic sublevels of energy states, which are, in the general case, coherently coupled to each other and take part in the radiation processes. Figure 1 gives a vivid presentation of the problem arising even in such a seemingly simple case when one need describe the radiation transitions caused by a strong monochromatic field between two energy levels with large values of the angular momentum J. If the field polarization is arbitrary, the whole set of the magnetic sublevels turn out to be coupled by radiative transitions. Formally, the problem becomes essentially multilevel. In this case not only the hope fades of solving it analytically using the traditional quantum-mechanical approach, but the problems of numerical solution grow abruptly with increasing quantum number J as well. On the other hand, as is often the case, every cloud has a silver lining. With large J we approach the situation when the rotational motion of particles can be described classically. It turns out that the transition from the quantum description of orientation states of the angular momentum to the classical one simplifies the problem radically: it reduces to the problem of radiation processes in the simplest model of nondegenerate states. In this case the rotational motion manifests itself in a dependence of the density matrix elements on orientation angles of the angular momentum as on a parameter.

DOI
10.1117/12.328232

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The behavior of a nonlinear oscillator (NO) coupled to a radiation field is investigated. The NO considered is an angular momentum oscillator, of energy $\ensuremath{\hbar}\ensuremath{\omega}{L}_{3}$, that describes the collective effect of a number of identical two-level (or spin-\textonehalf{}) systems under given idealized conditions, a large total angular momentum quantum number ${L}_{0}$ corresponding to a large number of two-level systems. The field is described by a set of modes. Free decay---with the NO initially excited and the radiation field in the ground state---and forced oscillation---with the NO subject to a prescribed resonant driving field---are studied. The analysis is performed both classically and quantum mechanically, using the classical and Heisenberg equations of motion, respectively, so as to display explicitly the difference in the results. 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Physical Review A•Sep 1, 1972•41 citations
In recent years interest has significantly quickened in investigation of nonlinear optical and spectroscopic phenomena in such unique objects as Rydberg atoms (the atoms in the energy states near the ionization limit) and van der Waals complexes (dimers). These objects are characterized, in particular, by that their energy states are strongly degenerate due to a large value of angular (rotational) momentum. Here, the problem arises of adequate theoretical description of experimental results, especially when polarization peculiarities of nonlinear radiation processes are considered. The problem is caused by the existence of a huge number of quantum magnetic sublevels of energy states, which are, in the general case, coherently coupled to each other and take part in the radiation processes. Figure 1 gives a vivid presentation of the problem arising even in such a seemingly simple case when one need describe the radiation transitions caused by a strong monochromatic field between two energy levels with large values of the angular momentum J. If the field polarization is arbitrary, the whole set of the magnetic sublevels turn out to be coupled by radiative transitions. Formally, the problem becomes essentially multilevel. In this case not only the hope fades of solving it analytically using the traditional quantum-mechanical approach, but the problems of numerical solution grow abruptly with increasing quantum number J as well. On the other hand, as is often the case, every cloud has a silver lining. With large J we approach the situation when the rotational motion of particles can be described classically. It turns out that the transition from the quantum description of orientation states of the angular momentum to the classical one simplifies the problem radically: it reduces to the problem of radiation processes in the simplest model of nondegenerate states. In this case the rotational motion manifests itself in a dependence of the density matrix elements on orientation angles of the angular momentum as on a parameter.
We generalize an approach (previously proposed by two of the authors) to describe quantum systems with large angular momentum exposed to a radiation field. The approach exploits a transformation from the quantum-mechanical description to the classical one with respect to angular momentum orientation. The transformation is carried out through a density matrix representation similar to the well known Wigner representation for the translational degrees of freedom. The generalization opens up the possibility of describing the interaction of polychromatic radiation (i.e. a set of monochromatic components) with a quantum system when the spectral components of the radiation are resonant to different transitions of the system. It follows naturally from the obtained equations that if the solution of the problem within the framework of the model of nondegenerate states is known, then its generalization for the case of state degeneracy and accounting for polarization of interacting fields is given by the simplest operation. As an example, the proposed method is applied to stimulated Raman scattering and four-wave mixing. We pay special attention to those polarization features which, on the one hand, are interesting to experimentalists and, on the other hand, have not yet been given an adequate explanation in the literature.
We develop a theory that describes the interaction of radiation and multilevel particles on the basis of the classical description of the orientation of angular momentum. For examples of application of this theory we take the problems of stimulated Raman scattering and of parametric generation of light in four-wave mixing. We find that the efficiency of the radiation processes largely depends on the polarization of the pump waves and on the types of optical transitions (Δ J ) and to a much lesser extent on the value of the angular momentum J . We also explain some polarization phenomena observed in experiments on four-wave mixing.
The numerical analyses of polarization phenomena is developed for the radiation fields resonant with the transitions nS1/2-nP1/2,3/2 and nP1/2,3/2 -- (n+2)S1/2 of alkaline atoms. The method of computer simulation of nonlinear resonant polarization phenomena is used, which is based on the solution of the problem of interaction of the real multilevel atom with two laser fields of arbitrary intensity and polarization and with a constant magnetic field. This method is known to be successful applied for the investigation of the polarization phenomena in the atomic gases of the alkaline atoms Na and K. In present paper the whole alkaline group is considered. The represented spectra of rotation of plane of polarization are appear to be qualitatively different for different atoms since atom fine- structure intervals differ very much from each other. The obtained spectra for Rb are in good agreement with the experimental spectra.
The theory and method of computer simulations created formerly permits to investigate the interaction of high power laser radiation up to gigawatt on centimeter to the second power with the atoms as well as with small so with large fine structure interval in the external magnetic field. The modifications of the energies and populations of atomic levels due to such interaction lead to the new nonlinear effects. Among them besides the modifications in Raman effect and new effects of rotation of plane of polarization and circular dichroism investigated before there are such new effects as the modifications of the number, intensities, polarizations of the lines at the excitation spectra and the scattering spectra of resonant fluorescence. The real atom is multilevel system. Usually the theoretical investigations of nonlinear resonant magnetooptical effects are limited by two- or three-level approximations or by using the perturbation theory. This is justified for considering the effects in the weak magnetic fields but not sufficient for revealing and investigation the characteristics of the new nonlinear magnetooptical effects taking place in the intense radiation and magnetic fields. Such effects are related to modifications of electronic structure of atoms (level shifts and splittings, populations modifications). As the considered media is atomic gas one can reach for power density up to gigawatt on centimeter to the second power. As the considered concentrations are small it is possible to neglect the collisional relaxation. For real atom the considered system is multilevel so only numerical solution is appropriated. The simulations permit to find some new effects in the excitation spectra of Raman effect and resonant fluorescence.
A class of bound-state problems which represent the interaction between a system of N two-level atoms and an electromagnetic radiation via an m-photon process is studied, with m = 1; 2; 3;.... We also evaluate some nonlinear effects usually related with the polarisability of the medium and with the dependence on the intensity of the radiation field on the matter-radiation interaction. We obtain exact values for the eigenstates and eigenvalues for all values of total angular momentum of the system and all possible number m of photons involved in the interaction. We give explicit analytic expressions for small numbers of atoms and discuss some aspects of the composition of the eigenstates and of the spectra obtained in these cases.
The behavior of a nonlinear oscillator (NO) coupled to a radiation field is investigated. The NO considered is an angular momentum oscillator, of energy $\ensuremath{\hbar}\ensuremath{\omega}{L}_{3}$, that describes the collective effect of a number of identical two-level (or spin-\textonehalf{}) systems under given idealized conditions, a large total angular momentum quantum number L0{L}_{0}L0​ corresponding to a large number of two-level systems. The field is described by a set of modes. Free decay---with the NO initially excited and the radiation field in the ground state---and forced oscillation---with the NO subject to a prescribed resonant driving field---are studied. The analysis is performed both classically and quantum mechanically, using the classical and Heisenberg equations of motion, respectively, so as to display explicitly the difference in the results. Interest in the comparison between the two formalisms is motivated by the expectation that for large L0{L}_{0}L0​, the NO should behave essentially classically, except near its highest-energy state in the absence of a driving field. The general equations of motion are reduced to equations for the NO variables only. In the classical analysis of free decay, expressions for the energy and oscillating coordinates are derived. The decay time is shown to approach infinity as L3(0){L}_{3}(0)L3​(0) approaches L0{L}_{0}L0​ (the limiting condition being that of unstable equilibrium) and the radiative frequency shift is shown to be approximately proportional to L3(t){L}_{3}(t)L3​(t). It is also shown that use of the rotating-wave approximation alters qualitatively the expression for the frequency shift. In the classical analysis of forced oscillation, approximate results are obtained for a weak driving field and a strong driving field, the NO being initially in the ground state. The weakfield results exhibit a monotonic approach of L3(t){L}_{3}(t)L3​(t) to a constant (negative) value---or steady state---at which the power absorbed equals the power radiated; in the strong-field case, L3(t){L}_{3}(t)L3​(t) oscillates periodically between the limits $\ifmmode\pm\else\textpm\fi{}{L}_{0}$, the coupling to the radiation field having negligible effect on the frequency of this oscillation. In the quantum-mechanical analysis, the equations of motion become simplified for L0=12{L}_{0}=\frac{1}{2}L0​=21​, and this case is treated first. The free-decay results are essentially similar to those of the Weisskopf-Wigner theory, exhibiting an exponential decay of 〈L3(t)〉〈{L}_{3}(t)〉〈L3​(t)〉 and a radiative frequency shift in the oscillating coordinates. Under forced oscillation, with $〈{L}_{3}(0)〉=\ensuremath{-}{L}_{0}, 〈{L}_{3}(t)〉$ approaches a constant value either monotonically, if the driving field is sufficiently weak, or by means of a damped oscillation, if the driving field is strong. For L0>12{L}_{0}>\frac{1}{2}L0​>21​, the free decay is treated by a method that involves the derivation of a set of expressions for the kthk\mathrm{th}kth derivative of 〈L3(t)〉〈{L}_{3}(t)〉〈L3​(t)〉 as an expectation value of a polynomial in L3{L}_{3}L3​ of order k+1k+1k+1. This set, together with the eigenvalue equation for L3{L}_{3}L3​, is shown to lead to a solution for all the moments of L3{L}_{3}L3​. The method is used to obtain complete solutions for several low values of L0{L}_{0}L0​, and also to obtain initial derivatives of 〈L3(t)〉〈{L}_{3}(t)〉〈L3​(t)〉 as polynomials in L0{L}_{0}L0​ for 〈L3(0)〉=L0〈{L}_{3}(0)〉={L}_{0}〈L3​(0)〉=L0​. For large L0{L}_{0}L0​, a comparison of classical and quantum-mechanical equations shows that only the condition $〈{L}_{3}(0)〉\ensuremath{\approx}{L}_{0}$ requires quantum-mechanical treatment, and that for a short time only. The free-decay problem with initial condition 〈L3(0)〉=L0〈{L}_{3}(0)〉={L}_{0}〈L3​(0)〉=L0​ solved quantum mechanically up to such a time t1{t}_{1}t1​ by means of the initial derivatives previously derived, and then this solution if used to provide initial conditions determining a classical solution for $t\ensuremath{\ge}{t}_{1}$. The statistical aspects introduced by the quantum mechanics are preserved in the classical solution, and their significance is discussed, with several examples, comparison is also made with a nonstatistical approximation. In the case of forced oscillation, the behavior of 〈L3(t)〉〈{L}_{3}(t)〉〈L3​(t)〉---for arbitrary L0{L}_{0}L0​---is examined in detail for a strong field, and turns out to be described by a damped oscillation, the existence of the damping being independent of L0{L}_{0}L0​. The apparent inconsistency of this result with the expectation that a large system subject to strong forces should behave classically is discussed, and 〈L23(t)〉〈{L}_{2}^{3}(t)〉〈L23​(t)〉 is examined. It is concluded that in a single experiment, the NO energy oscillates approximately like the classical energy, without damping; quantum mechanics introduces, however, a slight randomness (or unpredictability) in the frequency of this oscillation, because of the coupling with the radiation field. Since 〈L3(t)〉〈{L}_{3}(t)〉〈L3​(t)〉 describes the average over an ensemble of which each member consists of a NO coupled to a radiation field, the random frequency variation among the members accounts for the damping of the average. The usefulness of the combination of classical and quantum-mechanical analyses in achieving and interpreting theoretical results for a class of phenomena involving the collective interaction between a number of atoms and a radiation field is pointed out.