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Physical Review A

Coherent dynamics of N -level atoms and molecules. I. Numerical experiments

Joseph H. Eberly, Bruce W. Shore, Zofia Białynicka-Birula, Iwo Białynicki‐Birula

Published Nov 1, 1977• 108 citations
Publisher

Abstract

We study numerically the solution to Schr\"odinger's equation for the radiative interaction of fictitious $N$-level model atomic and molecular systems with monochromatic radiation fields. The numerical method of solution allows us to study multiphoton transitions in $N$-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.

DOI
10.1103/physreva.16.2038

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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 class of multiphoton-absorption problems has exact solutions. In these problems an NNN-level atom or molecule absorbs energy from near-resonance monochromatic laser fields, and one asks for the time-dependent populations of the energy levels of the absorber. We find that the equal-Rabi and the harmonic-Rabi NNN-level systems studied numerically in the preceding paper are associated with Chebyshev and Hermite polynomials. Using the exact solutions we find exact expressions for the time averages of occupation probabilities in terms of sums of squares of polynomials. In addition we find the first approximate analytic expression for the long-period population oscillations observed in numerical solutions; and we show that a steady-state population inversion between the highest and lowest levels may be maintained by multiphoton pumping.
Results are reported on coherent monochromatic multiphoton excitation in many-level systems, which are representative for some of the basic mechanisms for atomic and molecular multiphoton processes. Numerical solutions are discussed that use the Floquet and quasi-resonant approximations in the framework of the URIMIR program package. The excitation schemes include direct three-photon excitation, two-photon excitation with diagonal coupling, Göppert-Mayer-type two-photon processes, multiphoton excitation with off-resonant inter-mediates, and practically irreversible coherent excitation into dense spectral structures. Several interesting phenomena are observed, such as nonlinear line shifts and broadenings of multi-photon resonances of relevance for multiphoton spectroscopy and almost constant intermediate population inversions, potentially useful for laser design. The accurate numerical results are compared with approximate solutions from perturbation theory, and with simple analytical solutions from Rabi-type formulae.
The interaction of simple, two- and three-level atomic systems with monochromatic and nonmonochromatic laser radiation near resonance transitions is discussed based on the Schroedinger equation with radiation decay and no collisional relaxation, outside the framework of the usual perturbation theory. The mathematical schemes employed include the resonance approximation, exact methods, the quasi-energy method, the adiabatic approximation, etc. A large number of physical phenomena, such as oscillating and inverted populations, self-induced resonances, processes of first order in the weak field, Raman scattering, coherent population transfer, etc. are considered. The review is intended for a broad readership.
The Maxwell–Schrödinger equations describing the ultrashort laser pulse propagation in multilevel molecular media are shown to be analytically solvable and to reduce to nonlinear multisine-Gordon equations for certain models of the field–molecule system. Special cases of level schemes are shown to lead to soliton propagation. A numerical study is presented in order to examine the effect of nonresonant (virtual) transitions on pulse propagation and amplification in a three-level molecular system as a function of intensity and detuning.
Mathematical modeling of the population dynamics is performed for states of a three-level system (atom) with a V-type configuration transforming a light pulse. It is assumed that the excited eigenstates of the atom are degenerate and coupled by coherent interaction, one of the states being radiating (radiative), while the other state is nonradiating (“dark”). The population dynamics of atomic states is described on the basis of numerical solutions of equations for the matrix elements of the density operator. The dependence of the efficiency of population of the atomic dark state from the values of the parameters of an irradiation pulse and from the ratio of the period of population oscillations of excited atomic states (caused by their coherent interaction) to the lifetime of the atomic radiating state is determined. Typical examples of the time dependence of the population of states of the atom considered are presented for the cases of irradiation by a short (as compared to the lifetime of the radiating state) sinusoidal light pulse and by a long rectangular light pulse with the resonance carrier frequency.
We study the dynamics of an N-level atom coupled in a lossless cavity to a single-mode near-resonant quantized field. The atomic levels are coupled by the multiphoton transitions and the coupling constants between the field and the atomic levels are supposed to be intensity dependent. We find the exact solution for the state vector describing the dynamics of the atom-plus-field system. As an illustration we use the model for studying (i) the time evolution of the atomic occupation probability with the initially coherent field and (ii) the light squeezing, when the cavity field is initially in the vacuum state and the atom is prepared in the atomic ‘coherent state’ (a superposition of atomic states).