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Physical Review A

Nonlinear resonance effects in multilevel quantum systems weakly coupled to a thermal reservoir. II. Multiple-quantum transitions

Clayton W. Bates

Published Dec 1, 1974• 0 citations
Publisher

Abstract

This is the second in a series of three papers on nonlinear resonance effects in multilevel quantum systems in which quantum-mechanical systems are considered that are under the influence of any number of classically described driving fields (well defined in amplitude and phase) and are in weak contact with a thermal reservoir, such that relaxation may be described by means of phenomenological decay constants. In the first paper, referred to as I, a projection-operator formalism was developed for separating the equation of motion for the density operator into a part which may be treated by conventional time-dependent perturbation techniques and another part which, because it would give rise to secular terms using a time-dependent perturbation theory, must be treated by more exact means. In this paper three applications of the formalism developed in I are considered. The first application is to a system in which a multiple-quantum transition is taking place between two levels of the system which contains many levels between the two levels under consideration. In particular, the transition probability is calculated for these two levels, which are not directly connected by matrix elements of the interaction but are connected indirectly through intermediate states. The next application considered is the Raman effect in a four-level system. As a final application of the formalism developed in I an expression is derived for the magnetization ${M}_{+}(t)={M}_{x}(t)+i{M}_{y}(t)$ of a system of $N$ noninteracting spins under the influence of a static field in the $z$ direction and an arbitrary number of rf fields in the $x$ direction. As in I, a phenomenological form is assumed for the relaxation in all of these applications. It is shown in this problem that fields which are not involved in directly causing transitions in this system give rise to frequency shifts in the resonance conditions, which are accounted for in this treatment in a very natural and straightforward manner. For these fields, the rotating as well as the counter-rotating fields give shifts in the resonance condition.

DOI
10.1103/physreva.10.2360

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Nonlinear Resonance Effects in Multilevel Quantum Systems Weakly Coupled to a Thermal Reservoir

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Physical Review A•Jan 1, 1976•20 citations
This is the second in a series of three papers on nonlinear resonance effects in multilevel quantum systems in which quantum-mechanical systems are considered that are under the influence of any number of classically described driving fields (well defined in amplitude and phase) and are in weak contact with a thermal reservoir, such that relaxation may be described by means of phenomenological decay constants. In the first paper, referred to as I, a projection-operator formalism was developed for separating the equation of motion for the density operator into a part which may be treated by conventional time-dependent perturbation techniques and another part which, because it would give rise to secular terms using a time-dependent perturbation theory, must be treated by more exact means. In this paper three applications of the formalism developed in I are considered. The first application is to a system in which a multiple-quantum transition is taking place between two levels of the system which contains many levels between the two levels under consideration. In particular, the transition probability is calculated for these two levels, which are not directly connected by matrix elements of the interaction but are connected indirectly through intermediate states. The next application considered is the Raman effect in a four-level system. As a final application of the formalism developed in I an expression is derived for the magnetization M+(t)=Mx(t)+iMy(t){M}_{+}(t)={M}_{x}(t)+i{M}_{y}(t)M+​(t)=Mx​(t)+iMy​(t) of a system of NNN noninteracting spins under the influence of a static field in the zzz direction and an arbitrary number of rf fields in the xxx direction. As in I, a phenomenological form is assumed for the relaxation in all of these applications. It is shown in this problem that fields which are not involved in directly causing transitions in this system give rise to frequency shifts in the resonance conditions, which are accounted for in this treatment in a very natural and straightforward manner. For these fields, the rotating as well as the counter-rotating fields give shifts in the resonance condition.
Calculations are made to determine the response (power absorbed, magnetization, etc.) of a multilevel quantum system under the influence of any number of classically described driving fields (well defined in amplitude and phase). A nonperturbative theory is developed to account for those fields that are in resonance with the system. The nonresonant effects, such as virtual energy shifts, are included in the theory. We limit ourselves to a discussion of quantum systems that are in weak contact with a thermal reservoir. The procedure is the following A projection-operator formalism is developed which separates the density matrix of a system into two parts. One part is related to those portions of the driving fields that interact quite strongly with the system. The other part is the nonresonant or weakly interacting portion. An exact equation of motion, which includes the effects of the nonresonant part, is derived for the strongly interacting part of the density matrix. It is then shown that when relaxation can be represented by phenomenological decay constants, a unitary transformation can be found which reduces the equation of motion for the strongly interacting part of the density matrix so that an exact solution is possible. This solution is shown to give the major effects of the driving fields and can be used as the zeroth-order solution in a perturbation treatment of the whole density matrix. Frequency shifts such as the Bloch-Siegert shift and shifts due to couplings between the levels of interest (resonance levels) and other levels (nonresonance levels) all arise in the same natural way in our treatment. Our results in many instances are the extensions of the well-known results for a two-level quantum-mechanical systemm to an NNN-level one, and include resonant multiple quantum effects. As an example, a straightforward application of the method is carried out in order to compute the shifts in the resonance frequencies of a four-level system, driven by two oscillating fields connecting three of the levels, due to the counter-rotating components of the driving fields and the presence of the fourth level, which is not coupled to the other levels by the driving fields.
The multiple-linear-time-scale method is used to construct a perturbation theory for NNN-level quantum systems subjected to time-dependent perturbations. The secular and small-denominator terms which plague conventional time-dependent perturbation theory are avoided; consequently, the theory is useful for treating long-term behavior and resonant interactions. The introduction of a self-energy operator allows the shifts in energy levels to be displayed explicitly. When the perturbation is the dipole interaction with an electromagnetic field, the successive approximations yield the well-known rotating-wave approximation, corrections due to counter rotating terms, and the Bloch-Siegert frequency shift. The formalism is applicable to arbitrary pulse shapes, provided that $\ensuremath{\parallel}{H}_{1}\ensuremath{\parallel}\ensuremath{\ll}\ensuremath{\hbar}\overline{\ensuremath{\omega}}$, where $\ensuremath{\parallel}{H}_{1}\ensuremath{\parallel}$ represents the inter-action strength and $\overline{\ensuremath{\omega}}$ is a characteristic frequency of the field. Rabi oscillations induced by multiphoton resonances are automatically included, and this effect is demonstrated in the case of a square pulse with frequency approximately one half the resonance frequency for a transition between two vibrational levels of a molecule. These calculations are compared to an exact numerical solution in order to find the limits of validity of the approximation. Even at high intensities ($I\ensuremath{\sim}{10}^{14}$ W/cm2{\mathrm{cm}}^{2}cm2) the shifted resonance frequency is quite accurate; however, the approximate and exact solutions are slightly out of phase, so that the approximate solution can only be trusted for a few Rabi cycles. For much lower intensities ($I\ensuremath{\sim}{10}^{10}$ W/cm2{\mathrm{cm}}^{2}cm2), the approximate solution is valid for many thousands of Rabi cycles.
The application of transition operators ${\mathcal{P}}_{m,{m}^{\ensuremath{'}}}(t)=\mathrm{exp}(\mathrm{iHt})|m〉〈{m}^{\ensuremath{'}}|\mathrm{exp}(\ensuremath{-}iHt)$ is studied for the problem of an atomic system SSS with eigenstates m{m}m interacting with one or more damping reservoirs RRR. The average value of these operators gives the reduced density matrix ${{\ensuremath{\rho}}_{{m}^{\ensuremath{'}},m}}^{(S)}(t)$ for SSS. If RRR consists of broad-band distributions of harmonic oscillators, (e.g., radiative damping), then damped equations of motion can be derived for all ${\mathcal{P}}_{m,{m}^{\ensuremath{'}}}(t)$, even if SSS is a multilevel system. One need not specify the initial states of RRR, nor restrict the treatment to second order in the S-R coupling. The formalism is illustrated for the case where SSS consists of (i) a four-level atom in a resonant cavity (with broad-band modes also present), and (ii) a collection of atoms that can be treated as a multilevel spin system. Density-matrix equations are obtained for the case where no damping radiation is present initially. In (ii), the formalism is used to derive a two-time corrleation function without the aid of the fluctuation-regression theorem.
The matrix elements of the time-development operator are obtained exactly for the influence of many resonant or near-resonant fields on a system with a finite number of levels for arbitrary initial conditions in a wide class of problems. Perturbative techniques are presented which enable the exact treatment of all perturbations to a desired order. As examples, a three-level double-resonance and two eight-level triple-resonance systems are given. The applications of these exact solutions to the treatment of perturbations, including relaxation phenomena, are presented using both standard-perturbation-theory and density-matrix techniques.
The spontaneous radiative decay to the ground state of an atomic system initially in the higher of two excited states, coupled in a radiationless fashion by an external field, is investigated by the method of multiple-time-scale perturbation theory. The coupled differential equations of motion for the probability amplitudes are solved to second order, while the usual secular behavior of conventional time-dependent perturbation theory is eliminated in terms of two natural time scales: a fast time scale corresponding to the reciprocal of the level transition frequency and a slower time scale associated with the inverse of the radiation linewidth. Expressions are obtained to this order for the energy shifts and decay characteristics of the excited states and the energy distribution of the final-state photons, quantities previously determined by Fourier analysis and contour integration and by the phenomenological approach of Weisskopf and Wigner. A detailed comparison of these various methods of solution includes conditions under which the present results agree to second order with the previous calculations.
The effects of incoherent feeding and decay on a coherently driven two-level system are investigated using density-matrix techniques. A closed-form solution that includes the effects of relaxation and spontaneous emission between the two levels is obtained for cases in which the sample size is both small and large compared to the wavelength of the coherent field. The formalism developed herein is somewhat more general than the original approach of Bloch, Bloembergen, Purcell, Pound, and Redfield, insofar as it is applicable to cases where the trace of density matrix is not constant in time. As such, several new phenomena are predicted. Specifically, the steady-state solutions reveal that under appropriate conditions a significant off-resonance coherent component can be maintained indefinitely by the combination of driving field and incoherent feeding. We term this effect "kinetic coherence" and develop its formalism for both optical and radio-frequency fields.