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Acta Physica Slovaca Reviews and Tutorials

Coherent manipulations of atoms using laser light

Bruce W. Shore

Published Jun 1, 2008• 95 citations
Publisher

Abstract

Coherent manipulations of atoms using laser light The internal structure of a particle - an atom or other quantum system in which the excitation energies are discrete - undergoes change when exposed to pulses of near-resonant laser light. This tutorial review presents basic concepts of quantum states, of laser radiation and of the Hilbert-space statevector that provides the theoretical portrait of probability amplitudes - the tools for quantifying quantum properties not only of individual atoms and molecules but also of artificial atoms and other quantum systems. It discusses the equations of motion that describe the laser-induced changes (coherent excitation), and gives examples of laser-pulse effects, with particular emphasis on two-state and three-state adiabatic time evolution within the rotating-wave approximation. It provides pictorial descriptions of excitation based on the Bloch equations that allow visualization of two-state excitation as motion of a three-dimensional vector (the Bloch vector). Other visualization techniques allow portrayal of more elaborate systems, particularly the Hilbert-space motion of adiabatic states subject to various pulse sequences. Various more general multilevel systems receive treatment that includes degeneracies, chains and loop linkages. The concluding sections discuss techniques for creating arbitrary pre-assigned quantum states, for manipulating them into alternative coherent superpositions and for analyzing an unknown superposition. Appendices review some basic mathematical concepts and provide further details of the theoretical formalism, including photons, pulse propagation, statistical averages, analytic solutions to the equations of motion, exact solutions of periodic Hamiltonians, and population-trapping "dark" states.

DOI
10.2478/v10155-010-0090-z

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Coherent manipulations of atoms using laser light The internal structure of a particle - an atom or other quantum system in which the excitation energies are discrete - undergoes change when exposed to pulses of near-resonant laser light. This tutorial review presents basic concepts of quantum states, of laser radiation and of the Hilbert-space statevector that provides the theoretical portrait of probability amplitudes - the tools for quantifying quantum properties not only of individual atoms and molecules but also of artificial atoms and other quantum systems. It discusses the equations of motion that describe the laser-induced changes (coherent excitation), and gives examples of laser-pulse effects, with particular emphasis on two-state and three-state adiabatic time evolution within the rotating-wave approximation. It provides pictorial descriptions of excitation based on the Bloch equations that allow visualization of two-state excitation as motion of a three-dimensional vector (the Bloch vector). Other visualization techniques allow portrayal of more elaborate systems, particularly the Hilbert-space motion of adiabatic states subject to various pulse sequences. Various more general multilevel systems receive treatment that includes degeneracies, chains and loop linkages. The concluding sections discuss techniques for creating arbitrary pre-assigned quantum states, for manipulating them into alternative coherent superpositions and for analyzing an unknown superposition. Appendices review some basic mathematical concepts and provide further details of the theoretical formalism, including photons, pulse propagation, statistical averages, analytic solutions to the equations of motion, exact solutions of periodic Hamiltonians, and population-trapping "dark" states.
As light passes an atom, it exerts forces on the charges, electrons, and nuclei that alter the atomic structure. These may be slight distortions (perturbations) of the electron cloud or they may be more severe, as described in subsequent sections of this monograph. We wish to determine those changes, given the radiation field, or to devise a radiation field that will produce specified changes. The changes to the atomic structure also affect the radiation that subsequently passes the atom. To describe those effects we must consider wave equations for radiation in the presence of altered atomic structure. More generally we must find self-consistent equations for the atoms and the field together, as discussed in Chaps. 21 and 22. Here we consider mathematical descriptions of the influence of coherent radiation on individual atoms, molecules, or other single quantum systems. Individual atoms Traditional sources of emission and absorption spectra, though revealing energy states of the constituent atoms and molecules, are macroscopic samples. One observes averaged characteristics of many individual particles, see Chap. 16. Quantum theory offers the basic formalism for dealing with individual atoms exposed to controlled radiation fields. Several experimental techniques provide acceptable approximations to this ideal. The following paragraphs note some of these examples. Vapors Neutral atoms or molecules in a vapor move freely along straight-line paths, interrupted by brief collisions that redirect the two collision partners. When the kinetic energies of the two partners are small, there can be no transfer of kinetic energy into internal energy of either particle – the collision is elastic .
The quantum world within an atom or molecule that once attracted explorations only by academic physicists now provides fertile sustenance for chemists seeking control of chemical reactions and for engineers developing ever smaller electronic devices or tools for processing information with greater security. Whereas the first pioneers could only discover the most elementary properties – the discrete energy levels that characterize the internal structures of atoms and the radiative transitions that link these structures to our external world – it is now possible to alter that structure at will, albeit briefly. Objective This monograph presents the physical principles that describe such deliberately crafted changes, namely how single atoms or molecules (or other simple quantum systems) are affected by coherent interactions, primarily laser light – a subject that has been regarded first as a part of quantum electronics and then quantum optics but is most generally described as coherent atomic excitation [Sho90]. This physics has relevance to such basic concerns as the detection and quantitative analysis of trace amounts of chemicals, the catalysis or control of chemical reactions, the alignment of molecules, and the processing of quantum information. The physics necessarily involves elementary quantum mechanics, but it has many associations to the classical dynamics that governs macroscopic objects – waves and particles. The mathematics that quantifies the changes is that of differential equations, specifically coupled ordinary differential equations (ODEs), whose parameters incorporate the controls of experimenters and whose solutions, appropriately interpreted, quantify the resulting changes.
Theory of the interaction between atom and radiation field: three pictures in quantum mechanics description two-level atom and the optical Bloch equation quantized description of the radiation field Dicke Hamiltonian and Jaynes - Cummings model quantum theory of a small system coupling to a reservoir. The quantum properties of light: coherence of light squeezed states of light resonance fluorescence superfluorescence optical bistability effects of virtual photon processes. Quantum properties of the atomic behaviour under the interaction of the radiation field: collapses and revivals of the atomic populations squeezing effects of the atomic operators coherent trapping of the atomic population quantum characteristics of a two-atom system under the interaction of radiation field autoionization of the atom in a laser field motion of the atom in a laser field laser cooling.
Coherent excitation of an atomic excited state occurs during the propagation of near-resonant light pulses and is responsible for the induced polarization. Simultaneously, incoherent excitation occurs due to the relaxation processes described by the absorption coefficient. Here, the theory for the coherent and incoherent excitation is initially presented in terms of the traditional vector model. While a complete understanding of the two-level system is provided by the vector model, it is shown to be incomplete when the problem of directly monitoring the coherent and incoherent excitation is considered. This is because this latter problem involves more than two levels. For this more complicated multilevel problem, adiabatic states are introduced to gain further understanding. The adiabatic states are the stationary states of the atom in the presence of the near-resonant laser field; they help to explain the intimate connection between the coherent excitation and the two-photon resonance. Experimental measurements of the coherent and incoherent excitation associated with near-resonant pulse propagation in Rb vapor are presented. The double-resonance technique used a relatively strong pulsed dye laser tuned near the $5{S}_{\frac{1}{2}}\ensuremath{\leftrightarrow}5{P}_{\frac{1}{2}}$ transition (7948 \AA{}A) of Rb to produce the coherent and incoherent excitation, and a weak, tunable cw dye laser tuned in the region of the $5{P}_{\frac{1}{2}}\ensuremath{\leftrightarrow}6{D}_{\frac{3}{2}}$ transition (6206 \AA{}A) to monitor this excitation. In agreement with theory, the experimental results demonstrate that coherent excitation is responsible for two-photon absorption, while the incoherent excitation corresponds to one-photon absorption to the 5P125{P}_{\frac{1}{2}}5P21​​ state.
The major portion of this monograph discusses how given pulses of laser radiation affect individual atoms. This chapter inverts that relationship, describing how the matter alters the fields. Those field changes provide quantitative measures of the quantum-state changes produced in the atoms. Their description therefore is an adjunct to Chap. 19. Basically the incident radiation produces excitation which, in turn, alters the various multipole moments of the atoms. When viewed as a macroscopic sample of matter, such changes alter the electric polarization field P and the magnetization field M of the matter through which the radiation must pass. The Maxwell equations, see App. C.1, provide the needed description of how the P and M fields alter the electric and magnetic fields E and B . The combination of the Maxwell equations for the fields and the Schrödinger, Bloch, or Liouville equations for the atoms provide the tools needed to construct a self-consistent description of radiation passing through matter – atoms responding to a pulsed field and traveling waves being modified by the resulting atomic changes [All87; Ale92; Muk99; Die06; Vit01a]. The present chapter, drawing on [Sho90, Chap. 12] and App. C, discusses this theory. Incoherent radiation passing through matter typically undergoes exponential attenuation in accord with eqn. (6.9). A measure of the incremental change of intensity in distance L by absorption coefficient κ is the optical depth κ L . This parameter appears in rateequation treatments of incoherent light attenuation.
Descriptions of coherent excitation of multi-state quantum systems model changes through coupled ordinary differential equations that become more cumbersome as the number of involved quantum states increases. It is always useful to find simplifications of the equations, ideally involving exact analytic solutions. The ultimate simplification is to a set of independent pairs of quantum states. Such sets of independent two-state linkages occur naturally when we describe the excitation between two sets of degenerate Zeeman sublevels by a field that is linearly or circularly polarized. The Morris–Shore (MS) transformation, a Hilbert-space coordinate change, generalizes this procedure to replace the description of an elaborate linkage pattern of an -state Hamiltonian in the rotating-wave approximation by a set of independent two-state systems – a basis of paired bright states and excited states supplemented with dark states and spectator states. The three-state lambda-linkage found in stimulated Raman transitions is a simple example. Both bright and dark states have found application in various procedures for manipulating quantum states, either to achieve population transfer between states or to create coherent superpositions; the dark and spectator states coincide with particular dressed (or adiabatic) states. The present review describes the MS transformation, noting its historical background, and discusses examples of its use.