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Physical Review A

Analytical solutions for laser excitation of multilevel systems in the rotating-wave approximation

T. H. Einwohner, Jack Wong, J. C. Garrison

Published Oct 1, 1976• 51 citations
Publisher

Abstract

For a multilevel atom or molecule irradiated by a finite superposition of monochromatic fields, the time-dependent rotating-wave-approximation Schr\"odinger equation can be reduced to an eigenvalue problem when the detunings satisfy a consistency condition. This condition is analyzed and the reduction performed using a graph associated with the interaction Hamiltonian.

DOI
10.1103/physreva.14.1452

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For a multilevel atom or molecule irradiated by a finite superposition of monochromatic fields, the time-dependent rotating-wave-approximation Schr"odinger equation can be reduced to an eigenvalue problem when the detunings satisfy a consistency condition. This condition is analyzed and the reduction performed using a graph associated with the interaction Hamiltonian.
A strong laser field interacting with an atom or a molecule can induce a coherent process which includes a large number of energy levels. If we can find a transformation which eliminates the explicit time dependence of the interaction Hamiltonian (for example, the rotating-wave approximation), we can reduce the dynamic problem to the consideration of eigenvalues and eigenvectors of the Hamiltonian. However, the complexity of an arbitrary multilevel Hamiltonian usually forces us to use numerical methods, and, therefore, not much general understanding about multilevel systems can be achieved. We consider the multilevel problems in a more general setting. Our approach is based on the observation that an arbitrary Hamiltonian matrix can be transformed into a tridiagonal form by unitary transformation.1 A tridiagonal form represents a ladder-type multilevel system. From all W-level systems the ladder configuration is the simplest in the sense that the number of level connections is the smallest possible. This means that the most effective analysis of a given multilevel system can be achieved using the transformation to ladder configuration. The spectral analysis of ladders is facilitated by the connections to orthogonal polynomials and continued fractions. The investigations about the spectral properties of ladders are reported.
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 analyze the time-dependence of N-level systems under the Rotating Wave Approximation and dipole selection rules. Such systems can be solved straightforwardly if the Hamiltonian can be transformed into a time-independent form. The conditions under which a unitary transformation can be used to render time-dependent Hamiltonians into a time-independent form, thereby making the solution, are examined. After case-by-case analysis of different four and five-level systems, we conclude that systems having only one odd or even parity level achieve time-independence. In contrast, the others must satisfy a condition of laser detuning to achieve time-independence.
This paper is an extension of Fujii et al (quant--ph/0307066) and in this one we again treat a model of atom with n energy levels interacting with n(n-1)/2 external laser fields, which is a natural extension of usual two level system. Then the rotating wave approximation (RWA) is assumed from the beginning. To solve the Schr{\" o}dinger equation we set the {\bf consistency condition} in our terminology and reduce it to a matrix equation with symmetric matrix QQQ consisting of coupling constants. However, to calculate exp⁡(−itQ)\exp(-itQ)exp(−itQ) {\bfexplicitly} is not easy. In the case of three and four level systems we determine it in a complete manner, so our model in these levels becomes realistic. In last, we make a comment on Cavity QED quantum computation based on three energy levels of atoms as a forthcoming target.
In this article, by using the perturbation theory, we analytically solve the eigenvalue problem for the Hamiltonian describing the interaction of a Λ -type three-level atom with a single-mode radiation field without the rotating wave approximation (RWA). For this purpose, the atom–field interaction Hamiltonian, which contains the counter-rotating terms (CRTs), is transformed to an analytically solvable Hamiltonian by applying three successive unitary transformations. According to our calculations, the contribution of CRTs within the transformed Hamiltonian is in fact replaced by transforming the 'constant detuning' with the 'intensity-dependent detuning' in the first order, and the 'constant atom–field coupling' with the intensity-dependent coupling in the second order of the perturbation parameters. Then, by solving the eigenvalue problem for the transformed Hamiltonian, the eigenvector of the considered atom–field Hamiltonian is obtained analytically. Finally, after achieving the state vector of the atom–field system at an arbitrary time, a few nonclassical properties of the system state are investigated numerically. Meanwhile, we compare our results with the presence of RWA, from which the role of CRTs will be established.
The interaction of two continuous wave electric fields (lasers) with a two-level molecule, that has a nonzero difference d, between the permanent dipoles of the two states involved in a multiphoton two-color transition, is studied in the rotating wave approximation and by using exact methods. Analytical rotating wave approximation results for the time-dependent populations of the molecular states and for the resonance profiles are derived and used to help discuss the effects of permanent dipole moments in the two-color absorption problem. Several examples of multiphoton, two-color, two-level resonance profiles calculated in the rotating wave approximation and by using exact techniques, are employed for illustrative purposes. They are used to help quantify the conditions for the validity of the two-color rotating wave approximation, which are considerably more restrictive than the analogous conditions for the one-color rotating wave approximation with d≠0, and to illustrate the interpretive and predictive nature of the rotating wave approximation results. For example, there are many multiphoton, two-color transitions that are available if a molecule possesses permanent dipoles (d≠0). The analytic rotating wave approximation expression for the molecule-two laser coupling can often be used to reliably estimate the field parameters of the two lasers that are required to optimize a given transition relative to others.