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Molecular Physics

Multi-photon spectra in the presence of strongly saturating oscillating and static fields

J.V. Moloney, William J. Meath

Published Apr 1, 1978• 29 citations
Publisher

Abstract

A solution for the time-dependent Schrödinger equation is given for an N-level system interacting with a sinusoidal field of arbitrary amplitude , frequency v and phase δ, in the presence of an applied static field of arbitrary strength . The solution is obtained by a modification of a previous exact method of solution for and retains the essential analytic features of the exact wavefunction for the problem. The Floquet form of the solution yields (a) the location and the widths of allowed transitions and the location of forbidden transitions, by use of characteristic exponent plots, but without evaluating the spectrum, and (b) convenient expressions for the steady-state induced transition probabilities, including the effects of a uniform relaxation mechanism, that only require the solution of the wave equation over the initial period of the hamiltonian. The approach is equally applicable to Stark (or Zeeman) frequency sweep or tuning problems. The ability to incorporate the effects of static fields in the solution is important since a variety of problems (e.g. anti-crossing spectroscopy) involve the application of such fields to a level configuration interacting with a sinusoidal field. As a detailed specific example, the multi-photon steady-state induced transition probabilities and characteristic exponents are studied, as a function of frequency v, for the unperturbed and the perturbed two-level system under saturating conditions. It is also demonstrated, for the coupling strengths of interest in multi-photon calculations, that the method of solution discussed here is a viable unified alternative to dressed-atom techniques.

DOI
10.1080/00268977800100841

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An analytic expression for the absorption spectra of a two-level molecule or atom is derived, within the rotating wave approximation (RWA), which includes the effects of permanent dipole moments and static electric fields. The derivation is for the interaction of the system with a plane-polarized sinusoidal electromagnetic field (EMF) in the semi-classical electric dipole approximation. The RWA resonance profile, and a series of exactly calculated two-level model spectra, are used to investigate some single- and multi-photon spectral effects due to permanent dipoles and static fields, relative to the atomic problem (no permanent dipoles). These effects include the occurrence of even as well as odd photon transitions. Permanent dipole moments can cause narrowing of the resonances, oscillatory fringes around the resonances as a function of frequency, and decreases in the molecule-EMF coupling, relative to the atomic results. Comparisons with exact two-level model spectra are used to study the validity of the RWA results and indicate that several features, such as dynamic backgrounds and shifts of the resonance frequencies from the weak EMF limits of {dollar}\\omega\\sbsp{lcub}\\rm res{rcub}{lcub}\\rm N{rcub}{dollar} = {dollar}\\Delta{dollar}E/N, N = 1,2,3, dots, are missing in the RWA spectra as the coupling increases.;Perturbative corrections to the RWA absorption spectra and the full widths at half maxima for the resonances are derived, neglecting static fields, and used to investigate and explain the effects missing in the RWA; the RWA resonance profile is a zeroth plus first order result obtainable from a time-independent Floquet Hamiltonian secular equation. The usefulness and validity of the perturbative corrections are investigated and it is concluded that these corrections are not useful computationally past second order. However, the corrections are useful in understanding some of the deficiencies of the RWA. These include the shifts of the N-photon resonance positions to low frequency, with respect to {dollar}\\Delta{dollar}E/N, that can occur for molecules with non-zero permanent dipoles; the shift is always to high frequency for atoms. A series of exact model calculations, for "giant dipole" molecules, is also used to discuss the effects of permanent dipole moments on spectra and to establish comparisons with the recent literature on the subject.

•Jan 1, 1988•0 citations
A solution for the time-dependent Schrödinger equation is given for an N-level system interacting with a sinusoidal field of arbitrary amplitude , frequency v and phase δ, in the presence of an applied static field of arbitrary strength . The solution is obtained by a modification of a previous exact method of solution for and retains the essential analytic features of the exact wavefunction for the problem. The Floquet form of the solution yields (a) the location and the widths of allowed transitions and the location of forbidden transitions, by use of characteristic exponent plots, but without evaluating the spectrum, and (b) convenient expressions for the steady-state induced transition probabilities, including the effects of a uniform relaxation mechanism, that only require the solution of the wave equation over the initial period of the hamiltonian. The approach is equally applicable to Stark (or Zeeman) frequency sweep or tuning problems. The ability to incorporate the effects of static fields in the solution is important since a variety of problems (e.g. anti-crossing spectroscopy) involve the application of such fields to a level configuration interacting with a sinusoidal field. As a detailed specific example, the multi-photon steady-state induced transition probabilities and characteristic exponents are studied, as a function of frequency v, for the unperturbed and the perturbed two-level system under saturating conditions. It is also demonstrated, for the coupling strengths of interest in multi-photon calculations, that the method of solution discussed here is a viable unified alternative to dressed-atom techniques.
A previous exact formal and practical solution for the time-dependent Schrödinger equation for a two-level non-degenerate system in an arbitrarily strong sinusoidal field is transformed for an N-level system to a Floquet form. Using the Floquet form of the solution computationally convenient expressions are obtained for the phase and the phase-long time-averaged induced transition probabilities. The method exploits the time periodicity of the Schrödinger equation and the solution over the initial period of the hamiltonian provides all the information needed to obtain both the unaveraged and the averaged transition probabilities for the system. The method is illustrated by specific examples which are used to discuss some of the temporal features of the multi-photon spectra of two-level systems.
An exact method of solution to the time-dependent wave equation for a system interacting with a sinusoidal field, which formally treats time and the phase of the field on an equal footing, is used to discuss (1) the importance of averaging the properties of a system over the phase of the applied field and (2) the nature and behavior of the characteristic exponents derived from the Floquet solution (with particular emphasis on the frequency-sweep experiment). The results for the Zeeman tuning experiment are used to resolve recent discrepancies in the literature which relate to the validity of Shirley's important result for the two-level average induced transition probability involving the derivative of the characteristic exponents with respect to the Zeeman splitting parameter ${\ensuremath{\omega}}_{0}$. The explicit calculations included in this work are for the single-photon two-level problem. Important implications can be inferred from them with respect to both the importance of phase averaging and the usefulness of the characteristic exponents as a quantitative means of obtaining resonance frequency shifts and half-widths for multiphoton and multilevel problems.
A previously developed exact semiclassical method is used to evaluate multi-photon spectra and Floquet characteristic exponents (dressed-atom energies) for several multi-level systems interacting with both strong oscillating and static fields under varying degrees of saturation. The usefulness of characteristic exponent plots in extracting the physically significant features of the spectrum, without the necessity of evaluating portions of the complete spectrum, is demonstrated for a number of model three-level systems which are not directly amenable to study by the often used rotating-wave approximation. The effect of neighbouring non-resonant states on two-photon resonance profiles is also discussed using three to six level systems (H and Na atoms) as models.
Solutions of the time-dependent Schrödinger equation, in the semi-classical electric dipole approximation, are developed for the interaction of a two-level system, possessing both transition and diagonal dipole matrix elements, with applied static and sinusoidal electric fields. Exact solutions can only be obtained subject to conditions involving the orientations and strengths of the applied fields. These, and perturbative extensions, are used to discuss some of the features of multi-photon processes that depend on the existence of non-zero diagonal dipole matrix elements. Some of the results apply, in the limit of vanishing permanent moments, to the atomic two-level problem.
The problem of the interaction of a quantum system having discrete states, with a classical oscillating field, is reexamined as a problem in the solution of the time-dependent Schrodinger equation with a periodic Hamiltonian. A method is presented for approximating the time-dependent Hamiltonian with a time-independent one in the weak oscillating field case. With the aid of Floquet's theorem the problem is exactly converted to one with a time-independent Hamiltonian represented by an infinite matrix. The approximation of only two states then permits finding the resonance line shape by perturbation theory for both single and multiple quantum transitions with equal ease. The simple case of only two states connected by an off diagonal sinusoidal perturbation is studied in detail, and a complete description of the average transition probability is found for the strong oscillating field case. A few more complex cases are discussed. A deeper understanding of the analysis is obtained by examining the theory with the oscillating field quantized. Experimental verification of the theory could best be obtained by the methods of atomic beam spectroscopy at radio frequencies.
An analytic expression for the absorption spectra of a two-level molecule or atom is derived, within the rotating wave approximation (RWA), which includes the effects of permanent dipole moments and static electric fields. The derivation is for the interaction of the system with a plane-polarized sinusoidal electromagnetic field (EMF) in the semi-classical electric dipole approximation. The RWA resonance profile, and a series of exactly calculated two-level model spectra, are used to investigate some single- and multi-photon spectral effects due to permanent dipoles and static fields, relative to the atomic problem (no permanent dipoles). These effects include the occurrence of even as well as odd photon transitions. Permanent dipole moments can cause narrowing of the resonances, oscillatory fringes around the resonances as a function of frequency, and decreases in the molecule-EMF coupling, relative to the atomic results. Comparisons with exact two-level model spectra are used to study the validity of the RWA results and indicate that several features, such as dynamic backgrounds and shifts of the resonance frequencies from the weak EMF limits of {dollar}\\omega\\sbsp{lcub}\\rm res{rcub}{lcub}\\rm N{rcub}{dollar} = {dollar}\\Delta{dollar}E/N, N = 1,2,3, dots, are missing in the RWA spectra as the coupling increases.;Perturbative corrections to the RWA absorption spectra and the full widths at half maxima for the resonances are derived, neglecting static fields, and used to investigate and explain the effects missing in the RWA; the RWA resonance profile is a zeroth plus first order result obtainable from a time-independent Floquet Hamiltonian secular equation. The usefulness and validity of the perturbative corrections are investigated and it is concluded that these corrections are not useful computationally past second order. However, the corrections are useful in understanding some of the deficiencies of the RWA. These include the shifts of the N-photon resonance positions to low frequency, with respect to {dollar}\\Delta{dollar}E/N, that can occur for molecules with non-zero permanent dipoles; the shift is always to high frequency for atoms. A series of exact model calculations, for "giant dipole" molecules, is also used to discuss the effects of permanent dipole moments on spectra and to establish comparisons with the recent literature on the subject.