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Physical Review

Self-Coupling of a Two-Level System by a Mirror

Hans Morawitz

Published Nov 25, 1969• 229 citations
Publisher

Abstract

We discuss, from a classical as well as a quantum-mechanical point of view, the effect of the coupling of an excited two-level system with itself due to emission and absorption of electric-dipole radiation, the emitted radiation being reflected by a nearby mirror. Expressions familiar from resonance-scattering theory are found for the shift of the transition frequency and linewidth from their values in the absence of the mirror. This renormalization effect leads to spatial modulation in the transition frequency and width of the excited state due to its resonant interaction with itself via the radiation field reflected from the mirror. This formalism is applied to some recent experiments with monomolecular dye layers. The experimental values of the fluorescence lifetime are in good agreement with the theory for distances from 500 to 6000 \AA{}.

DOI
10.1103/physrev.187.1792

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We discuss, from a classical as well as a quantum-mechanical point of view, the effect of the coupling of an excited two-level system with itself due to emission and absorption of electric-dipole radiation, the emitted radiation being reflected by a nearby mirror. Expressions familiar from resonance-scattering theory are found for the shift of the transition frequency and linewidth from their values in the absence of the mirror. This renormalization effect leads to spatial modulation in the transition frequency and width of the excited state due to its resonant interaction with itself via the radiation field reflected from the mirror. This formalism is applied to some recent experiments with monomolecular dye layers. The experimental values of the fluorescence lifetime are in good agreement with the theory for distances from 500 to 6000 \AA{}.
A simple theoretical model is formulated which describes dynamical features of the interaction of two-level atoms with a continuum of radiation oscillators. In particular, this paper is concerned with resonance scattering by single atoms in the presence of an external classical field, and spontaneous emission by a system of identical atoms. In the case of resonance scattering, the response of an atom to rapid changes of the amplitude of the external field is studied. The model for spontaneous emission by a system of atoms is based on the assumptions that all atoms have the same resonance frequency, and that the atoms are contained in a volume whose extension is small compared with the wavelength of the emitted radiation. The complete evolution of a system of mmm atoms is determined by a set of coupled first-order linear differential equations, and explicit solutions are presented for the values m=1,2,3,4,and8m=1,2,3,4, \mathrm{and} 8m=1,2,3,4,and8. Pair correlations of the atoms and photon-number fluctuations are discussed. An approximation for resonance fluorescence by a system of atoms with a broad distribution of resonance frequencies is included in an Appendix.
The effect of collisions on the resonance fluorescence spectrum of two-level atoms excited by monochromatic resonance radiation is studied. Analysis is performed for systems where the Doppler broadening is small compared to the collision frequency (high buffer gas pressures) and for the general case where collisions arbitrarily change the phase of the radiation-induced dipole moment (from completely interrupted to completely unaffected phase of the dipole moment). Both at a relatively low and at a high excitation radiation intensity, the resonance fluorescence spectrum is shown to depend on whether the two-level system is closed or open. This is especially true for the narrow unshifted Rayleigh scattering line. It is shown that, although the absorption line is homogeneously broadened, the resonance fluorescence spectrum exhibits a clearly pronounced anisotropy. In a direction close to the direction of propagation of the excitation radiation, the Rayleigh scattering line is maximally narrowed. Under certain conditions (that can easily be created in experiments), the width of this line is proportional to the diffusion coefficient of atoms interacting with the radiation.
We study analytically the effect of the dipole-dipole interaction on the statistics of the fluorescent radiation emitted from a system of two two-level atoms resonantly driven by a coherent field. For some interatomic separations, an inhibition of fluorescence occurs, which is reminiscent of the recently discussed quantum-jump phenomenon in a single three-level atom. This is reflected in the behaviors of the intensity correlation function, Mandel's Q parameter, and the time-dependent fluorescence spectrum. It is argued that this quantum-jump-like behavior arises from the coupling between the symmetric states and the antisymmetric state caused by the dipole-dipole interaction.
The calculation is given of the spectral distribution of resonance fluorescence from an atom that is driven near a j=12j=\frac{1}{2}j=21​ to j=12j=\frac{1}{2}j=21​ transition by a monochromatic, xxx-polarized electric field and that is subject to radiation damping only. In accordance with Mollow's results for a two-level system, the power spectrum of the scattered radiation corresponding to the xxx component of the dipole moment contains a coherent part for all driving-field intensities. The coherent part is absent in the fluorescence radiation corresponding to the yyy and zzz components of the dipole moment. For weak driving fields all power scattered by these latter components is present in a narrow Lorentzian. Consistent with energy conservation, the width of the Lorentzian corresponds to the probability of excitation of the atom out of its ground level due to the presence of the driving field. For strong driving fields the power spectra corresponding to the xxx component and to the yyy or zzz component mainly differ in the heights and widths of their central incoherent band and their Rabi-precession-frequency-shifted side bands.
The photon correlations of resonance fluorescence emitted by a degenerate two-level atom near a metal surface are studied. An intense nonmonochromatic optical laser drives a low-lying atomic transition, and the emitted fluorescence is detected by a photon counter. An expression for the spontaneous-decay operator is derived, and it appears that the various substates of the upper level have a different lifetime due to the presence of the surface, or equivalently, due to the loss of spherical symmetry. The temporal photon correlation function is then evaluated in terms of a photon-emission operator and the time-evolution operator for the atomic density matrix. The general theory is exemplified with a detailed elaboration of the jg{j}_{g}jg​=0\ensuremath{\rightarrow}je{j}_{e}je​=1 transition, for which the two-photon correlation is obtained explicitly as a function of the inverse lifetime A(h), depending on the atom-surface distance h, the laser linewidth, the detuning from resonance, and the dipole-coupling strength with the external field.