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Physical Review A

Adiabatic following in multilevel systems

J. Oreg, F. T. Hioe, Joseph H. Eberly

Published Feb 1, 1984• 421 citations
Publisher

Abstract

The problem of achieving population inversion adiabatically in an $N$-level system using one or more laser fields whose detunings and/or amplitudes are continuously varied is studied analytically and numerically. The $\mathrm{SU}(N)$ coherence vector picture is shown to suggest unexpected inversion procedures and also to give a generalized interpretation of adiabatic following. It is shown that the (${N}^{2}\ensuremath{-}1$)-dimensional $\mathrm{SU}(N)$ space contains an ($N\ensuremath{-}1$)--dimensional steady-state subspace $\mathit{\ensuremath{\Gamma}}(t)$ whose orthonormal basis vectors ${\stackrel{\ensuremath{\rightarrow}}{\ensuremath{\Gamma}}}_{1},\dots{}, {\stackrel{\ensuremath{\rightarrow}}{\ensuremath{\Gamma}}}_{N\ensuremath{-}1}$ are given explicitly in terms of the Hamiltonian matrix elements. The motion of the system can be interpreted as a "generalized precession" of $\stackrel{\ensuremath{\rightarrow}}{\mathrm{S}}$ about $\mathit{\ensuremath{\Gamma}}$. Multilevel adiabatic following occurs when the angle $\ensuremath{\chi}(t)$ between the coherence vector $\stackrel{\ensuremath{\rightarrow}}{\mathrm{S}}$ and its projection onto $\mathit{\ensuremath{\Gamma}}$ is very small. The multiple dimension of $\mathit{\ensuremath{\Gamma}}$ is shown to provide a variety of paths for adiabatic inversion. The adiabatic solution is obtained by solving $N\ensuremath{-}1$ simple equations for the directional cosines of $\stackrel{\ensuremath{\rightarrow}}{\mathrm{S}}$ on ${\stackrel{\ensuremath{\rightarrow}}{\ensuremath{\Gamma}}}_{i}$. The adiabatic solution and time scale and the state taken up by the atomic variable are discussed analytically and numerically for a three-level system.

DOI
10.1103/physreva.29.690

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The problem of achieving population inversion adiabatically in an NNN-level system using one or more laser fields whose detunings and/or amplitudes are continuously varied is studied analytically and numerically. The SU(N)\mathrm{SU}(N)SU(N) coherence vector picture is shown to suggest unexpected inversion procedures and also to give a generalized interpretation of adiabatic following. It is shown that the (N2\ensuremath−1{N}^{2}\ensuremath{-}1N2\ensuremath−1)-dimensional SU(N)\mathrm{SU}(N)SU(N) space contains an (N\ensuremath−1N\ensuremath{-}1N\ensuremath−1)--dimensional steady-state subspace \ensuremathΓ(t)\mathit{\ensuremath{\Gamma}}(t)\ensuremathΓ(t) whose orthonormal basis vectors \ensuremathΓ\ensuremath→1,…,\ensuremathΓ\ensuremath→N\ensuremath−1{\stackrel{\ensuremath{\rightarrow}}{\ensuremath{\Gamma}}}_{1},\dots{}, {\stackrel{\ensuremath{\rightarrow}}{\ensuremath{\Gamma}}}_{N\ensuremath{-}1}\ensuremathΓ\ensuremath→​1​,…,\ensuremathΓ\ensuremath→​N\ensuremath−1​ are given explicitly in terms of the Hamiltonian matrix elements. The motion of the system can be interpreted as a "generalized precession" of S\ensuremath→\stackrel{\ensuremath{\rightarrow}}{\mathrm{S}}S\ensuremath→​ about \ensuremathΓ\mathit{\ensuremath{\Gamma}}\ensuremathΓ. Multilevel adiabatic following occurs when the angle \ensuremathχ(t)\ensuremath{\chi}(t)\ensuremathχ(t) between the coherence vector S\ensuremath→\stackrel{\ensuremath{\rightarrow}}{\mathrm{S}}S\ensuremath→​ and its projection onto \ensuremathΓ\mathit{\ensuremath{\Gamma}}\ensuremathΓ is very small. The multiple dimension of \ensuremathΓ\mathit{\ensuremath{\Gamma}}\ensuremathΓ is shown to provide a variety of paths for adiabatic inversion. The adiabatic solution is obtained by solving N\ensuremath−1N\ensuremath{-}1N\ensuremath−1 simple equations for the directional cosines of S\ensuremath→\stackrel{\ensuremath{\rightarrow}}{\mathrm{S}}S\ensuremath→​ on \ensuremathΓ\ensuremath→i{\stackrel{\ensuremath{\rightarrow}}{\ensuremath{\Gamma}}}_{i}\ensuremathΓ\ensuremath→​i​. The adiabatic solution and time scale and the state taken up by the atomic variable are discussed analytically and numerically for a three-level system.
We derive and discuss the behavior of several multilevel models relevant to the problem of molecular multiphoton excitation under the action of a quasimonochromatic laser field, the amplitude of which rises slowly and falls rapidly on a certain internal time scale. Our method is suitable for the numerical solution of problems involving the adiabatic excitation of large multilevel systems. We find adiabatic inversion to be a general characteristic of the models considered. The fact that adiabatic inversion is accompanied by marked qualitative and quantitative changes in the expectation value of the dipole operator makes our results useful for understanding the propagation of laser pulses. An explicit expression that is especially convenient for numerical evaluation is presented for determining the limiting internal time scale, which is determined by the energy levels and transition moments of the system and the laser frequency. We illustrate the criterion for adiabatic inversion by applying it to a particular multilevel model. From a density-matrix treatment we conclude that collisional damping destroys the coherence required for adiabatic inversion. On the basis of our results we believe that the adiabatic approximation may be appropriate for some experiments of current interest.
A numerical analysis is presented of several potential pulsed-laser applications of adiabatic population inversion in atoms or molecules. A simple numerical method is demonstrated for evaluating adiabatic processes in multilevel systems for both swept-frequency and resonant, time-delayed pulses. Adiabatic inversion with time-delayed pulses is generalized to systems with any number of levels. The effect of Doppler broadening on time-delayed adiabatic pumping of a three-level system is investigated.
A systematic investigation of N-level inversion schemes, with use of ``chirped frequency lasers,'' in and beyond the adiabatic limit is presented. (1) It is shown that, contrary to intuition, the favorable scheme for adiabatic inversion requires that, during the process, resonances occur in reversed order, i.e., first the (N-1)-N transition and then backward along the atomic-level ladder down to the transition 1-2. (2) A new multilevel inversion process at fast rates (far beyond the adiabatic limit) is found. Surprisingly, the process occurs for pulse area equal to \ensuremath{\pi} in spite of large (time-dependent) detunings. Full analytic explanation of this generalized \ensuremath{\pi} pulse inversion is presented. General new properties of the multilevel adiabatic approximation are also derived and discussed.
A precessing vector model has been developed for the geometrical interpretation of the adiabatic following and the optimal detuning methods, which play a decisive role in coherent population transfer in a three-level system. In our model, the Bloch vector defined by a population inversion and two-photon coherence components precesses about the torque vector consisting of an effective Rabi frequency and detuning components. The Bloch vector traces out different routes depending on combinations of the time delay of two laser pulses and detunings from the resonant frequencies. For the extreme cases where the optimal detuning with zero delay and the optimal delay with zero detunings are taken, our vector model with analytical solutions is compared with numerical solutions.
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.