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Canadian Journal of Physics

The driven quantum-mechanical two-level system: small fields and long relaxation times

J. E. Grindlay

Published Jan 1, 1987• 0 citations
Publisher

Abstract

A formal theory of the long-term response of a dissipative two-level quantum-mechanical system to a monochromatic applied electric field is used to describe the fundamental and third-harmonic resonances in the small-field and long relaxation-times regime. Resonance frequencies, including Bloch–Siegert shifts, and resonance amplitudes for the dipole-moment components and the upper level probability function are obtained. A comparison with the rotating-wave approximation is made.

DOI
10.1139/p87-014

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A formal theory of the long-term response of a dissipative two-level quantum-mechanical system to a monochromatic applied electric field is used to describe the fundamental and third-harmonic resonances in the small-field and long relaxation-times regime. Resonance frequencies, including Bloch–Siegert shifts, and resonance amplitudes for the dipole-moment components and the upper level probability function are obtained. A comparison with the rotating-wave approximation is made.
The shifted frequency approximation is used to solve the equations of motion for the density matrix describing a quantum mechanical two-level system, with decay, in an applied monochromatic electric field. Expressions are obtained for the transient and the long-term linear electric dipole moment and occupation probability, and the long-term third-order dipole moment. The results are valid across the frequency spectrum, including resonance, provided the phenomenological decay times for the system are not too large or too close in value.
A two-level dissipative quantum-mechanical system subjected to a small applied multimode electric field plus a feedback term proportional to the induced dipole moment is discussed. The long-term behaviour of the induced dipole moment and of the upper level occupation probability is represented by a series expansion in terms of the applied electric-field amplitudes. First-order and third-order internal, external, and intrinsic polarizabilites are introduced and calculated for the model. Certain ratios of third-order to first-order polarizabilities are shown to have a common value for the internal, external, and intrinsic cases. Clausius–Mossotti relations for the linear and third-order susceptibilities are derived.
A power-series expansion for long-time solutions is obtained for the density-matrix equations of motion describing a quantum-mechanical two-level system with dissipation and feedback. The resonances in the first- and third-order dipole contributions and the second-order upper level occupation probability are shown to be significantly affected by the feedback.The results are applied to the case of a uniformly polarized, finite, crystalline dielectric made up of two-level systems. Polarizabilities relating the dipole moment to each of the applied field, the internal field, and the macroscopic field are introduced and relations between them derived. The dipole-moment – macroscopic-field polarizabilities are shown in particular to be shape independent. Susceptibilities are defined and related to the single-system polarizabilities through generalized Clausius–Mossotti relations.
Previously derived equations for the expectation values of the dynamical variables of a general two-level dipole system (TLS) coupled to a relaxation mechanism---of which the Bloch equations for a spin-\textonehalf{} magneticdipole system are a special case---are reformulated in the density-matrix formalism in order to point out the explicit difference in the relaxation terms between the present description, which includes electric-dipole systems, and that of conventional treatments that are based on the assumption that any TLS is equivalent to a spin-\textonehalf{} magnetic dipole. The original equations are then solved for a weak monochromatic driving field, and the frequency of maximum power absorption is shown to depend on the type of TLS under consideration. The case of a stronger monochromatic driving field and the resulting saturation effects are studied for a special TLS, a spatially linear electric dipole which may have permanent dipole moment. This case exhibits a strong-field resonance shift that depends on the magnitude of the permanent dipole moment. A driving field consisting of a strong component at resonance and a weak component near resonance is considered in connection with the same TLS. The polarization is shown to contain, in lowest order, a component at the difference frequency with an amplitude determined by the magnitude of the permanent dipole moment.
The time evolution of a two-level system interacting with a classical monochromatic radiation field is calculated by Fourier transforming the equations of motion. This can be done exactly if one uses the convolution of the product of two Fourier transformations. The method produces recurrence relationships for the transforms. The time-dependent amplitudes of the states and the transition probability are evaluated by using two such recurrence relationships. The time-averaged probability shows characteristic resonances at odd multiples of the ratio of the natural frequency of the system to the frequency of the radiation field. The peaks of the resonances are displaced by the Bloch-Siegert shift. At these resonances the system is completely saturated with the flipping frequency dependent on the strength of the radiation field. The time dependence and the frequency spectrum of the dipole moment is determined at the main resonance and at the three-quantum resonance. The spectrum contains the zero-frequency terms which are responsible for the coherence resonances.
Previous theory describing the behavior of a general two-level system (TLS) coupled to a loss mechanism and driven by an oscillating field near resonance is generalized to include an arbitrary driving field. Integro-differential equations of motion for the expectation values of the Pauli spin matrices, which describe completely the behavior of a TLS, are derived. The relaxation constants involved in these equations prove to be frequency-dependent, and reactive effects produced by the loss mechanism appear. It is shown that for an approximately monochromatic driving field near resonance, the general equations of motion can be approximated by differential equations. In the case of a magnetic TLS, these differential equations reduce to the Bloch equations if reactive effects are neglected. An exact solution of the general equations of motion for the special, simple case of a magnetic TLS being driven by a transverse rotating field of arbitrary frequency is obtained, and deviation from a Lorentzian resonance shape, caused by the frequency dependence of the relaxation and reactive constants, is found to exist.