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Physical Review A

Two-photon near-resonance scattering of a time-dependent light beam

M. Kolwas

Published Mar 1, 1980• 2 citations
Publisher

Abstract

Time-dependent spectra of light emitted after two-photon excitation with nonresonant intermediate state are studied by the perturbation method. Two components are distinguished: a slow one ${I}_{s}$ connected with the excited-state population, and a fast one ${I}_{f}$ connected with the double-quantum optical coherence. For large detuning of the two-photon frequency from the excited-ground-state energy separation, the fluorescent light is found to be ${I}_{s}\ensuremath{-}|{I}_{f}|$, and the Raman-scattered light is ${I}_{f}$. The influence of statistics of light, laser linewidth, spectral bandwidth of the detector, and transfer of coherence from the ground to the excited state are also taken into consideration.

DOI
10.1103/physreva.21.902

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Coherent four-photon scattering of light due to excited and autoionizing states of atomic systems is considered. We analyze the influence of one-photon resonances at the frequency of the anti-Stokes signal and at the frequency of the pump wave on the shape of the spectrum of four-photon scattering. We derive analytical expressions for the line shapes of four-photon scattering involving one-photon resonances with allowance for phase-matching conditions and variation in the populations of excited states for limiting regimes of tight focusing and strong absorption in a medium with a cubic nonlinearity. The calculated spectra of four-photon scattering include the interference of resonant and nonresonant components of the third-order nonlinear susceptibility with allowance for one-photon saturation. We develop a method for normalizing experimental spectra of four-photon scattering with one-photon resonances that takes into account distortion of spectral lines due to the influence of phase mismatch and one- photon absorption.
The review deals with various variants of classification of the types of secondary emission of light by molecules; cases are distinguished in which the secondary emission occurs without additional processes that find their way between photon emission and absorption; the advisability of differentiating between the cases of resonance fluorescence and resonance scattering is noted. Reference is made to papers that have made contributions to the development of quantum-mechanical and classical theory of Raman scattering and to the development of the concepts of the relations between electron-vibrational absorption spectra, fluorescence spectra, and scattering excitation near and near and far resonance. Conditions are considered of excitation of the spectrum at different relations between the electronic-oscillator damping constant, the atom vibration frequency, the rotational frequencies, and the difference between the frequency of the incident light and the frequency of the electronic transition. The conditions for the excitation of typical light scattering, typical resonance fluorescence, and certain intermediate types, in which individual features of scattering are combined with certain features of fluorescence (phenomena of the transition type) are noted. The results of investigations of different models of the scattering centers, their advantages, shortcomings, and limits of applicability are compared. The most interesting results of the experimental investigations of resonant scattering of light by molecules and crystals are noted.
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Two-time correlations in the emissions of photons by a single atom of sodium in the presence of a coherent exciting field near resonance have been investigated. In the experiment sodium atoms in an atomic beam are excited by a perpendicular light beam from a tunable dye laser, and they are prepared by optical pumping to behave as two-level quantum systems. The fluorescent light is collected by a microscope objective in a direction that is approximately orthogonal to both beams and imaged on two photomultipliers. Photoelectric pulse correlations are measured in the presence of exciting fields of various strengths and for various detunings from the atomic resonance, and are found to exhibit significant nonclassical features. The results show clearly that the emitted photons exhibit antibunching, in good quantitative agreement with the predictions of quantum electrodynamics.