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Proceedings of the Royal Society of London A Mathematical and Physical Sciences

Theory of dispersion in relation to light shifts

S. Pancharatnam

Published Oct 3, 1972• 4 citations
Publisher

Abstract

Abstract A quantum mechanical system consisting of one photon interacting with N atoms not far from resonance is considered and an (approximately) stationary solution found for the eigenstates and energy of the interacting system. It is shown that the interaction energy (light shift) is simply related to the atomic polarizability. A consideration of the expectation value of the operator representing the first-order correlation function of an optical field yields a quantum-mechanical interpretation of refractive index.

DOI
10.1098/rspa.1972.0145

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Abstract A quantum mechanical system consisting of one photon interacting with N atoms not far from resonance is considered and an (approximately) stationary solution found for the eigenstates and energy of the interacting system. It is shown that the interaction energy (light shift) is simply related to the atomic polarizability. A consideration of the expectation value of the operator representing the first-order correlation function of an optical field yields a quantum-mechanical interpretation of refractive index.
Classical dispersion theory Many aspects of the interaction between radiation and matter can be described quite accurately by a classical theory in which the medium is represented by model atoms consisting of positive and negative parts bound by an attraction which depends linearly on their separation. Although quantum theory is necessary to calculate from first principles the magnitude of the parameters involved, in this chapter we shall show that many optical effects can be interpreted physically in terms of this model by the use of classical mechanics. In §13.5 we shall relax the restriction of linearity. Some of the quantum mechanical foundations will be discussed briefly in Chapter 14, but most are outside the scope of this book (see Yariv, 1989; Loudon, 1983). The term dispersion means the dependence of dielectric response (dielectric constant and refractive index) on frequency of the wave field. This will be the topic of the present section. Afterwards we shall see some of the applications of dielectric response to spatial effects. The classical atom Our classical picture of an atom consists of a massive positive nucleus surrounded by a light spherically-symmetrical cloud of electrons with an equal negative charge. We imagine the two as bound together by springs as in Fig. 13.1, so that in equilibrium the centres of mass and charge of the core and electron charge coincide. As a result the static atom has zero dipole moment.
Abstract The dispersion relation is obtained for a system of four-level atoms with an equidistant energy spectrum, which interact with resonant laser radiation, with account for three sequential one-photon optically allowed transitions, two-photon transitions, as well as a direct three-photon transition. It is shown that the dispersion relation consists of four polariton branches. The divergence and convergence of the dispersion relation branches, their intersection, and a self-consistent change in the binding force of photons with atoms are predicted using the fixed photon concentration approximation.
Quantum-mechanical expressions for nonresonance-dipole light-scattering cross sections are related to corresponding expressions for oscillator strengths and refractive indices. In particular, Rayleigh and Raman cross sections for atoms are expressed in terms of oscillator strengths and vector-coupling coefficients. Several of our results, including the relationship between Rayleigh scattering and refractive index, differ in general from the corresponding results of classical dispersion theory. We show that these differences arise from antisymmetric components Ckja = (Ckj − Cjk)/2 of the polarizability tensor, which have been neglected in the classical analyses. Calculated Rayleigh cross sections for cesium and aluminum atoms, and Raman cross sections for aluminum atoms are presented to illustrate our results. The antisymmetric contribution is found to be substantial in all of these cross sections; its most obvious effect is to cause the depolarization (for linearly polarized incident light) to exceed 34 over extended wavelength ranges away from resonance. On the other hand, for atoms initially in states of zero angular momentum, and molecules under conditions which allow the use of Placzek’s polarizability approximation, our results agree with those of classical dispersion theory.
The problem of resonant interaction between an electromagnetic radiation field and a vibronic system, such as a molecule or a localized electronphonon system, is considered. The vibronic coupling is assumed to result from displaced and distorted potential energy surfaces for the vibrational motion in the electronic quantum states involved in the resonant interaction with the radiation field. Furthermore, the vibrational energy relaxation is taken into account without assumptions about Markovian-type relaxation. In order to study correlation properties of higher than second order in the electric field strength of the light emitted a method of calculation of the expectation value of an arbitrary product combination of effective time evolution operators of the vibronic system is developed. The calculations are performed by utilizing Feynman's disentangling and operator ordering techniques and yield closed solutions in the low-temperature limit. The theory is used for studying the intensity and the normally ordered intensity correlation function of the resonance fluorescence light from a two-atom molecule excited by a relatively weak laser field, which undergoes phase fluctuations. It is shown that the vibronic coupling can give rise to an anticorrelation effect which is substantially stronger than in the case of resonance fluorescence from an atom. For the case of small vibrational damping a general formula which directly connects the asymptotic long-time behaviour of the normalized intensity correlation function with the vibrational relaxation in the molecule is deduced. It should be convenient for the determination of very small vibrational decay rates.
The refractive index of a system is often viewed as the collective response of a medium to an electromagnetic field. Nevertheless, even if targeted at a single atom, the incoming light undergoes the dispersion. By studying the propagation of a single photon interacting with a two-level atom, we examine the dispersion behavior, calculate the phase and group velocity of the photon wave packet, and further analyze the dispersion experienced by the photon. These findings are critical for advancing long-distance quantum communications.