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John Wiley & Sons, Inc. eBooks

Quantum Interference in Atomic and Molecular Systems

Z. Ficek

Published Apr 2, 2003• 6 citations
Publisher

Abstract

In this review the author discusses the major effects resulting from the modification of spontaneous emission by quantum interference. He begins in Section II by presenting elementary concepts and definitions of the first- and second-order correlation functions, which are frequently used in the analysis of the interference phenomena. Section III describes the master equation approach used for analyzing quantum interference effects in atomic and molecular systems. In Sections IV and V the author reviews the fundamental quentum interference effects in spontaneous emission and in coherently driven systems. He discusses different schemes for suppression of spontaneous emission and population trapping and gives an alternative explanation of these effects in the dressed-atom picture. Section VI deals with the problem of amplification on dark transitions, which are important for information processing without spontaneous emission. The effect of quantum interference on photon correlations is discussed in Section VII. Multilevel systems composed of two transitions with parallel dipole moments and methods for generating two transitions with nonorthogonal dipole moments are briefly discussed in Section VIII. The final section (Section IX) deals with the experimental demonstration of constructive and desctructive interference effects in a driven molecular system.

DOI
10.1002/0471231479.ch2

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Journal of Modern Optics•Feb 21, 2006•2 citations
In this review the author discusses the major effects resulting from the modification of spontaneous emission by quantum interference. He begins in Section II by presenting elementary concepts and definitions of the first- and second-order correlation functions, which are frequently used in the analysis of the interference phenomena. Section III describes the master equation approach used for analyzing quantum interference effects in atomic and molecular systems. In Sections IV and V the author reviews the fundamental quentum interference effects in spontaneous emission and in coherently driven systems. He discusses different schemes for suppression of spontaneous emission and population trapping and gives an alternative explanation of these effects in the dressed-atom picture. Section VI deals with the problem of amplification on dark transitions, which are important for information processing without spontaneous emission. The effect of quantum interference on photon correlations is discussed in Section VII. Multilevel systems composed of two transitions with parallel dipole moments and methods for generating two transitions with nonorthogonal dipole moments are briefly discussed in Section VIII. The final section (Section IX) deals with the experimental demonstration of constructive and desctructive interference effects in a driven molecular system.
We discuss the connection between quantum interference effects in optical beams and radiation fields emitted from atomic systems. We illustrate this connection by a study of the first- and second-order correlation functions of optical fields and atomic dipole moments. We explore the role of correlations between the emitting systems and present examples of practical methods to implement two systems with non-orthogonal dipole moments. We also derive general conditions for quantum interference in a two-atom system and for a control of spontaneous emission. The relation between population trapping and dark states is also discussed. Moreover, we present quantum dressed-atom models of cancellation of spontaneous emission, amplification on dark transitions, fluorescence quenching and coherent population trapping.
Quantum interference and coherence effects in the interaction of atoms with the quantized electromagnetic field are investigated theoretically. A general master equation for the description of atom-field interactions is introduced. The interplay of the concepts of complementarity and interference in the time-energy domain are studied on the basis of the fluorescence light emitted by a single laser-driven atom, where the coherence of spontaneous processes gives rise to quantum interference in the spectrum of resonance fluorescence. The vacuum-induced dipole-dipole interaction in pairs of multi-level atoms is analyzed. It is shown that the interaction between orthogonal transition dipole moments of different atoms does not only influence the system dynamics crucially, but implies that the few-level approximation in general cannot be applied to near-degenerate Zeeman sublevels of the atomic level scheme. Potential applications of dipole-dipole interacting multi-level atoms for the implementation of decoherence-free subspaces and the generation of entanglement between atomic states are examined. The generation of an entangled state of the radiation field with a macroscopic number of photons is discussed on the basis of a single-atom laser.
It has been observed experimentally [H.R. Xia, C.Y. Ye, and S.Y. Zhu, Phys. Rev. Lett. 77, 1032 (1996)] that quantum interference between two molecular transitions can lead to a suppression or enhancement of spontaneous emission. This is manifest in the fluorescent intensity as a function of the detuning of the driving field from the two-photon resonance condition. Here we present a theory that explains the observed variation of the number of peaks with the mutual polarization of the molecular transition dipole moments. Using master equation techniques we calculate analytically as well as numerically the steady-state fluorescence, and find that the number of peaks depends on the excitation process. If the molecule is driven to the upper levels by a two-photon process, the fluorescent intensity consists of two peaks regardless of the mutual polarization of the transition dipole moments. If the excitation process is composed of both a two-step, one-photon process and a one-step, two-photon process, then there are two peaks on transitions with parallel dipole moments and three peaks on transitions with antiparallel dipole moments. This latter case is in excellent agreement with the experiment.
A general expression for the spectrum of cascade spontaneous emission from an arbitrary multilevel system is presented. Effects of the quantum interference of photons emitted in different transitions are analyzed. These effects are especially essential when the transition frequencies are close. Several examples are considered: (i) Three-level system; (ii) Harmonic oscillator; (iii) System with equidistant levels and equal rates of the spontaneous decay for all the transitions; (iv) Dicke superradiance model.
We study the spontaneous-emission properties of a coherently driven four-level atom, and show a few interesting phenomena such as fluorescence quenching, spectral-line narrowing, spectral-line enhancement, and spectral-line elimination. These phenomena can be observed in experiment since the rigorous condition of near-degenerate levels with nonorthogonal dipole moments is not required here. Qualitatively, these phenomena can be attributed to the quantum interference between competitive spontaneous-decay channels in the bare-state picture or the spontaneously generated coherence between two close-lying levels in the dressed-state picture.
Second-order interference effects in the spontaneous emission by two identical two-level atoms, separated a distance apart and both initially excited, are considered. On the basis of the analysis in our previous paper published in 2004, within fourth-order perturbation, detailed analysis of the second-order quantum interference in the emitted field is made. The interference arises both from single-photon states and two-photon states owing to interferences between different decaying sequences. By detailed analysis we have found some cancellations between single-photon and two-photon interference terms, and an interpretation of this is given. The contributions from the single- and the two-photon states as well as the total interference are analysed numerically for various interatomic distances and times. The contribution from a two-photon state is mostly larger than that from a single-photon state except when the atomic electric dipole is large, in which case the two contributions can be comparable. It is shown that the emission patterns from the two interacting atoms provide more information on atom–atom correlations than the decay time evolution of the atomic states population does. The number of interference fringes and the distance between them depend on the interatomic distance in a similar fashion to Young's interference fringes.