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Physical Review A

Coherent dynamics of N -level atoms and molecules. IV. Two- and three-level behavior

Bruce W. Shore, Richard J. Cook

Published Nov 1, 1979• 29 citations
Publisher

Abstract

The authors demonstrate special cases for which the resonantly excited $N$-level atom displays particularly simple periodic behavior involving only two levels. The cases, which occur when first and last transitions are weak, have analytic solutions. A striking difference is noted between even-$N$ and odd-$N$, related to the resonance structure of the dressed ($N\ensuremath{-}2$)-level atom.

DOI
10.1103/physreva.20.1958

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Fluorescence intensity and squeezing in a driven three-level atom: Ladder case

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A theoretical study is made of the steady-state intensity and squeezing properties of the fluorescent light from a three-level-atom system in a ladder configuration, which is subject to spontaneous-emission decay to the electromagnetic-field vacuum. Two cases are examined: in the equispaced (ES) level case, the two atomic transition frequencies are nearly equal and two photon absorption processes occur from a single coherent laser field that couples both transitions and has a small detuning from each; in the non- equispaced (NES) level case, the atomic transition frequencies are rather different and two photon absorption processes occur from two coherent laser fields, each coupled to a single transition and in near resonance with it. In both cases, a situation of small two-photon detuning occurs. Optical Bloch equations for the atomic density matrix in rotating frames are given and matrix expressions for determining the steady-state populations and coherences are obtained. Analytic expressions are also given for special cases. The fluorescent intensity is obtained from the populations of the intermediate and upper states, with the normally ordered variance (NOV) for quadrature components of the fluorescent field involving, in addition, the atomic coherences. The fluorescent intensities are shown graphically as a function of two-photon detuning for a variety of one-photon detunings and Rabi frequencies for the ES and NES cases.In both cases, the fluorescent intensities show the well known resonances from the upper state at zero two-photon detuning and from the intermediate state at zero one-photon detuning for the lower transition. However, further resonances are also found. The intermediate-state intensity displays a resonance at zero two-photon detuning. Also, the upper-state intensity shows a resonance at zero one-photon detuning for the upper transition, but only for the NES case; evidently, the transfer rate from upper to lower transition coherences destroys this resonance for the ES case. The time-averaged NOV is also shown graphically as a function of two-photon detuning for a variety of one-photon detunings and Rabi frequencies for the ES and NES cases. For the ES case, the quadrature frequency is chosen as the single laser frequency and for the NES case, it is chosen as either the average of the two laser frequencies or the lower transition laser frequency. Squeezing occurs near zero two-photon detuning for both ES and NES cases, though only for the quadrature frequency equal to the average laser frequency in the latter case. It also occurs near zero detuning for the lower transition for both cases, though only for the quadrature frequency equal to the lower transition laser frequency in the NES case. The squeezing minima show a splitting effect for large Rabi frequencies corresponding to two-photon or one-photon Rabi splitting of the dressed atom levels for the situation near two-photon or one-photon resonance, respectively. The large squeezing near two-photon resonance for moderate Rabi frequencies and large one-photon detuning corresponds to essentially pure three-level squeezing, while that near one-photon resonance for weak Rabi frequencies involves two-level squeezing.

Physical Review A•May 1, 1995•62 citations
The authors demonstrate special cases for which the resonantly excited NNN-level atom displays particularly simple periodic behavior involving only two levels. The cases, which occur when first and last transitions are weak, have analytic solutions. A striking difference is noted between even-NNN and odd-NNN, related to the resonance structure of the dressed (N\ensuremath−2N\ensuremath{-}2N\ensuremath−2)-level atom.
By employing an analogy with a spin-JJJ system in a constant magnetic field the authors obtain a simple soluble model for stepwise laser excitation of an NNN-level system (N=2J+1N=2J+1N=2J+1), including analytic treatment of Doppler detuning and of ionization loss. The solutions are periodic and hence permit complete population inversion. A simple graphical realization of the population dynamics, a generalization of the Feynman, Vernon, and Hellwarth vector model of the two-level Bloch equation, is then described.
Previously published papers have noted the existence of two-level periodicities in idealized theoretical models of monochromatic excitation of multilevel systems. The present paper provides a theoretical derivation of such two-level dynamics from the more general NNN-level rotating-wave-approximation Schr\"odinger equation and applies the resulting formulas to different extremes of excitation in a nondegenerate system of sequential (ladderlike) excitation: first, when intermediate levels have much larger cumulative detunings than Rabi frequencies, and second, when intermediate Rabi frequencies are much larger than detunings. In each case one has simple analytic expressions for the effective two-level Rabi frequencies and detunings.
We study numerically the solution to Schr\"odinger's equation for the radiative interaction of fictitious NNN-level model atomic and molecular systems with monochromatic radiation fields. The numerical method of solution allows us to study multiphoton transitions in NNN-level systems unhampered by the assumptions usually adopted, such as weak fields or large detunings of intermediate states, in perturbative and quasiperturbative analytic studies. We point out regularities and near regularities in the population dynamics that appear to be qualitatively different from those encountered in two- and three-level systems.
We show that a simple nonperturbative two-level model of an atom driven by a very strong periodic field, results in a rich picture of very high harmonic generation and related phenomena. It reproduces experimentally observed plateau, yields for the first time simple analytic formulas for the plateau cutoff frequency, critical driving intensity, and saturation, and predicts intensity-induced multi-resonances. One of the most fascinating phenomenon discovered recently in nonlinear interaction of light with atoms and ions, is very high-order (up to 135) odd harmonic generation (HHG) by intense (∼ 1013 W/cm2 and higher) optical laser radiation in rare gasses and some ions [1], The spectra of generated harmonics drasticly deviate from the perturbation theory predictions [2], In particular, intensity of harmonics, falling monotonically with their orders only up to a certain point, levels off forming a so-called “plateau", and falls monotonically again beyond it. Generally, harmonte generation depends on phase-matching conditions and nonlinear response of individual atoms. It has recently become clear however [3,4] that the major features of HHG, in particular the plateau, result mainly from general properties of atomic nonlinear response. The most direct and apparently successful way so far to approach the problem theoretically has been numerical simulation of the Schrödinger [2,5-7] (including an empiric rule [6]) for many-electron atoms using Hartry-Slater approximation. This approach requires, however, tremendous amount of calculations and involves many processes, making it difficult to gain simple insights. An interesting simplified model [8] based on 3-D delta-potential with a single (ground) level [9] produces results in integration form. The idea of retaining a single energy scale (ionization energy) brings one close to an even simpler system: a two-level model atom. A two-level model of HHG [10], however, due to various complications introduced into it, failed to generate simple results, whereas an analytic solution [11] holds for a virtually degenerate two-level model only (see below) which is unapplicable to the experimental conditions [1-4,7,9]; besides, no relaxation was considered in [10,11].
A theoretical study is made of the steady-state intensity and squeezing properties of the fluorescent light from a three-level-atom system in a ladder configuration, which is subject to spontaneous-emission decay to the electromagnetic-field vacuum. Two cases are examined: in the equispaced (ES) level case, the two atomic transition frequencies are nearly equal and two photon absorption processes occur from a single coherent laser field that couples both transitions and has a small detuning from each; in the non- equispaced (NES) level case, the atomic transition frequencies are rather different and two photon absorption processes occur from two coherent laser fields, each coupled to a single transition and in near resonance with it. In both cases, a situation of small two-photon detuning occurs. Optical Bloch equations for the atomic density matrix in rotating frames are given and matrix expressions for determining the steady-state populations and coherences are obtained. Analytic expressions are also given for special cases. The fluorescent intensity is obtained from the populations of the intermediate and upper states, with the normally ordered variance (NOV) for quadrature components of the fluorescent field involving, in addition, the atomic coherences. The fluorescent intensities are shown graphically as a function of two-photon detuning for a variety of one-photon detunings and Rabi frequencies for the ES and NES cases.In both cases, the fluorescent intensities show the well known resonances from the upper state at zero two-photon detuning and from the intermediate state at zero one-photon detuning for the lower transition. However, further resonances are also found. The intermediate-state intensity displays a resonance at zero two-photon detuning. Also, the upper-state intensity shows a resonance at zero one-photon detuning for the upper transition, but only for the NES case; evidently, the transfer rate from upper to lower transition coherences destroys this resonance for the ES case. The time-averaged NOV is also shown graphically as a function of two-photon detuning for a variety of one-photon detunings and Rabi frequencies for the ES and NES cases. For the ES case, the quadrature frequency is chosen as the single laser frequency and for the NES case, it is chosen as either the average of the two laser frequencies or the lower transition laser frequency. Squeezing occurs near zero two-photon detuning for both ES and NES cases, though only for the quadrature frequency equal to the average laser frequency in the latter case. It also occurs near zero detuning for the lower transition for both cases, though only for the quadrature frequency equal to the lower transition laser frequency in the NES case. The squeezing minima show a splitting effect for large Rabi frequencies corresponding to two-photon or one-photon Rabi splitting of the dressed atom levels for the situation near two-photon or one-photon resonance, respectively. The large squeezing near two-photon resonance for moderate Rabi frequencies and large one-photon detuning corresponds to essentially pure three-level squeezing, while that near one-photon resonance for weak Rabi frequencies involves two-level squeezing.