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Soviet Journal of Quantum Electronics

Fluorescence spectrum of a multilevel atom under two-photon resonance conditions

B. A. Grishanin, Fred H. Schmidt

Published Oct 31, 1981• 0 citations
Publisher

Abstract

It is shown that, under two-photon resonance conditions in a strong electromagnetic field, a strong quantum coupling may be observed between two-photon and one-photon transitions and this coupling results in new physical effects. Calculations are made of the corresponding fluorescence spectrum at the frequency of a two-photon dipole-forbidden transition.

DOI
10.1070/qe1981v011n10abeh008414

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It is shown that, under two-photon resonance conditions in a strong electromagnetic field, a strong quantum coupling may be observed between two-photon and one-photon transitions and this coupling results in new physical effects. Calculations are made of the corresponding fluorescence spectrum at the frequency of a two-photon dipole-forbidden transition.
We consider the possible physical processes that may arise in a three-level atom when only two of its levels interact with a strong electromagnetic field and when the atomic transition frequency is nearly equal to once and twice the frequency of the laser field, respectively. There have been found pronounced cooperative effects in the spectrum of the two-level system, which is in resonance with the laser field, arising from the presence of the third level. The excitation spectra describing the transitions from the first excited state into the second excited state and from that to the ground state consist, apart from the two central peaks, of two pairs of sidebands which are induced by the laser field of the neighbouring system. Detailed expressions of the spectral functions for the physical processes of one- and two-photon resonance fluorescence have been derived and discussed in the limit of high photon densities. The excitation spectrum of the low frequency modes has been considered and discussed in detail. It is found that quantum beats in spontaneous emission may appear in the spectra of the one- and two-photon resonance fluorescence arising from the interference between the two atomic transition frequencies and the frequency of the laser field. The importance of the low frequency modes that occur in the processes in question has been pointed out.
We have studied the fluorescence spectra arising from the interaction of a three-level atom with two strong electromagnetic fields whose initially populated modes are equal to the two atomic transition frequencies, respectively. The Green's function formalism has been used to calculate the excitation spectrum of the system. An expression for the spectral function describing the excitation spectrum of the system has been derived in a closed form in the limit of high photon densities. Numerical computation of the expression for the spectral function indicates that at each transition frequency there may exist either one pair or two pairs or three pairs of sidebands, in addition to the central peak, depending upon the relative strength of the Rabi frequencies involved.
We present a theory of two-photon resonance fluorescence of an atom or molecule in which the excitation by an external electromagnetic field as well as fluorescence emission is mediated by two-photon processes. The treatment is based on first dressing the atom or molecule by the external field and then evaluating perturbatively the effect of the interaction with the vacuum or fluorescent field and so resonance fluorescence can be considered as spontaneous emission from the dressed atom. The introduction of the combined system of atom and external field via dressed states leads to simpler calculations and more transparent physics. The fluorescence spectrum derived by us has similarities as well as differences with that of one-photon resonance fluorescence and earlier theoretical predictions for the two-photon case.
The excitation spectrum arising from the interaction between two identical atoms (molecules), one of which is excited in the presence of a resonant strong electromagnetic field (pump field), is investigated. The excitation spectrum is found to consist of those describing the symmetric and antisymmetric modes, respectively. The form of both spectra depends on the relation between the distance RRR separating the atoms and the wavelength $\ensuremath{\lambda}$ of the transition from the ground state to the excited state. For $R<\ensuremath{\lambda}$, and when certain conditions prevail, the spectral function for the symmetric modes consists of three Lorentzian lines describing the central peak and the two sidebands whose radiative widths are equal to ${\ensuremath{\gamma}}_{0}$, $\frac{3{\ensuremath{\gamma}}_{0}}{2}$, and $\frac{3{\ensuremath{\gamma}}_{0}}{2}$, which are twice the corresponding ones arising from an isolated single atom interacting with the pump field. For the antisymmetric modes the central peak has a $\ensuremath{\delta}$-function distribution indicating the stability of the mode in question, while, when certain conditions are satisfied, the two sidebands are described by Lorentzian lines each having a radiative width of the order of $\frac{{\ensuremath{\gamma}}_{0}}{2}$, which is equal to the natural linewidth for a photon spontaneously emitted from an isolated atom. For both the symmetric and antisymmetric modes, the dipole-dipole interaction between the atoms brings about small energy shifts. For $R>\ensuremath{\lambda}$, apart from the small energy shifts caused by the dipole-dipole interaction, the spectral functions for symmetric and antisymmetric modes are similar to that for the single atom interacting with the pump field.