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Soviet Physics Uspekhi

Resonance interaction of intense light with atoms

Nikolai B. Delone, В. П. Крайнов

Published Apr 30, 1978• 9 citations
Publisher

Abstract

Some typical resonance nonlinear-optics phenomena taking place when light interacts with atoms are considered. The multitude of such phenomena reduces to scattering of the perturbing light, perturbation of the atomic spectrum, excitation of an atom and its ionization. In all these cases the investigations are carried out using the simplest model—an isolated atom in a monochromatic external field. Such a model enables one to give an exact description of many elementary processes. On the other hand it is sufficiently realistic. A detailed investigation is carried out of resonance fluorescence, spontaneous Raman scattering, multiphoton excitation of atoms, resonance shifts and splitting of atomic levels and resonance lonication of atoms. The nature of these processes is investigated as a function of the intensity of the external field, its frequency, a specific atomic spectrum, the nature of polarization of the perturbing field, and the degree of its nonlinearity. The role played by the field of the electromagnetic vacuum is analyzed. Theoretical predictions are compared with the results of many experiments describing resonance processes of the interaction of an intense light field with atoms.

DOI
10.1070/pu1978v021n04abeh005539

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Some typical resonance nonlinear-optics phenomena taking place when light interacts with atoms are considered. The multitude of such phenomena reduces to scattering of the perturbing light, perturbation of the atomic spectrum, excitation of an atom and its ionization. In all these cases the investigations are carried out using the simplest model—an isolated atom in a monochromatic external field. Such a model enables one to give an exact description of many elementary processes. On the other hand it is sufficiently realistic. A detailed investigation is carried out of resonance fluorescence, spontaneous Raman scattering, multiphoton excitation of atoms, resonance shifts and splitting of atomic levels and resonance lonication of atoms. The nature of these processes is investigated as a function of the intensity of the external field, its frequency, a specific atomic spectrum, the nature of polarization of the perturbing field, and the degree of its nonlinearity. The role played by the field of the electromagnetic vacuum is analyzed. Theoretical predictions are compared with the results of many experiments describing resonance processes of the interaction of an intense light field with atoms.
The most important results of study of multiphoton ionization of atoms are reviewed. Discussions are presented of specific features of the process, theoretical methods of description of ionization of atoms in a strong light field, the basic principles of design of experiments in which intense laser radiation is used, results of investigation of direct and resonance processes of multiphoton ionization, and the mutual relation between multiphoton processes (multiphoton excitation and ionization) and various phenomena leading to perturbation of the spectrum of bound states of an electron in an atom under the influence of a strong light field.
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 splitting of the line of resonance scattered light from atomic systems, being a mong the most interesting phenomena in resonance nonlinear optics has received considerable attention during the past decade [1–11]. It is known by now that the number of lines into which the spontaneous scattered light spectrum splits, grows up with increasing the number N of strongly coupled atomic (or molecular) levels as N(N-1)+1 [10, 11]. But while the character of resonance fluorescence (RF) from a two- and three-level systems has been extensively studied [1–91], the number of papers devoted to the spectral structure of scattered light from systems with N>3 is scarce. In reality there is only one work [12], known to us, which treat s certain aspects of the spectrum of RF from a four-level system irradiated by three strong light fields at exact resonance.
The review describes and interprets the basic phenomena recently observed in the interaction between free atoms and laser radiation. Some of these have been known for a long time in magnetic resonance but in the optical range, the situation is strongly modified because of spontaneous emission and the Doppler effect. Therefore, particular attention is paid to resonance fluorescence and Doppler-free spectroscopy but without dwelling on applications. Transient effects are also discussed, but all the phenomena which characterize, not specifically the interaction between atoms and fields, but the free evolution of atoms after coherent excitation are ignored. Pulse propagation experiments are described in detail and multiphoton processes are considered, with special emphasis on Doppler-free multiphoton excitation and resonant multiphoton ionization.
A detectable nonlinear response between light and matter depends on one of two key ingredients: Either there is a resonance between the light wave and some natural oscillation mode of the material, or the light is sufficiently intense. In this chapter, the authors let the matter variables themselves play active roles and derive coupled nonlinear differential equations for the electric and matter fields. They outline the use of Schrodinger's equation to derive the Bloch equations, which describe the dynamics of the oscillators of matter and help to derive the Maxwell equation for the envelope of an almost monochromatic electromagnetic wave. The authors analyse the case of two distinct co- or counter-propagating waves interacting with a three-level medium where both waves excite separate quantum transitions sharing a common level. They also help to derive an effective two-level atom model that describes two-photon absorption and stimulated Raman scattering.
The phenomenon of resonance fluorescence provides an interesting manifestation of the quantum theory of light and is a “real world” application of the material of the Chapters 8 and 9. In this process, a two-level atom is typically driven by a resonant continuous-wave laser field and the spectral and quantum statistical properties of the fluorescent light emitted by the atom are measured. Experimentally this can be achieved by scattering a laser off a collimated atomic beam such that the directions of the laser beam, atomic beam, and detector axis are mutually perpendicular as shown in Fig. 10.1. If the driving field is monochromatic, then at low excitation intensity the atom absorbs a photon at the excitation frequency and reemits it at the same frequency as a consequence of conservation of energy. The spectral width of the fluorescent light is therefore very narrow. The situation, however, is considerably more complicated when the excitation intensity increases and the Rabi frequency associated with the driving field becomes comparable to, or larger than, the atomic linewidth. At such intensity levels, the Rabi oscillations show up as a modulation of the quantum dipole moment and sidebands start emerging in the spectrum of the emitted radiation. This so-called dynamic Stark splitting is an interesting feature of the atom–field interaction. In addition to that, the fluorescent light exhibits certain nonclassical properties including photon antibunching and squeezing. In this chapter, we develop a theory of resonance fluorescence to explain these phenomena.