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In the preceding chapters, we discussed the manipulation and observation of atomic variables associated with the internal degrees of freedom. A complete separation between internal and external degrees of freedom, like position and momentum, is not always possible, however. It therefore appears appropriate to include a discussion of the mechanical effects of light, which have received increasing attention in recent years. The transfer of momentum between photons and atoms, first observed more than sixty years ago, had to wait for the wide availability of lasers to become a useful experimental tool. In particular the cooling of atoms and atomic ions to very low temperatures has found numerous applications.
Light-induced forces
That light exerts mechanical forces on massive particles like atoms may appear surprising. To motivate the existence of such an effect two different approaches are possible. The first approach considers the light as a collection of photons that carry, apart from energy and angular momentum, linear momentum as well. Photons interacting with atoms can therefore change the momentum of the atoms. The second approach considers light as a wave, i.e., an inhomogeneous electromagnetic field interacting with the atomic dipole moment. Both approaches provide a possible description for the numerous phenomena that can occur in this context, but in many situations, one of them turns out to be more intuitive or more useful for calculations than the other.
After the sequence of introductory chapters that collected the necessary tools, we are now ready to discuss complete experiments. The first type of experiment we consider is the creation and detection of order in multilevel atoms through coherent Raman processes. The atoms that we use to study these processes are rare earth ions in a crystal matrix. Enclosing them in a crystal allows long interaction times, but also makes it necessary to consider their interaction with neighbouring atoms.
Overview
Raman processes
Introduction
In the preceding chapters, we mentioned several types of Raman processes. Their common feature is a resonant change of the energy of the photons that interact with the material system. The energy of the scattered photons may be lower (Stokes process) or higher (anti-Stokes) than that of the incident photons. The energy difference is transferred to the material system, where it must match an energy level separation. The photon energy itself, however, does not have to match exactly a transition frequency of the medium. This is commonly expressed by the statement that the Raman scattering proceeds through a virtual state, represented by the dashed line in Figure 7.1. The presence of a real state of the atom, indicated by the full line, nevertheless increases the coupling efficiency, as discussed in Chapter 3.
The earlier sections on three-level effects and optical anisotropy dealt with the mathematical formalism of Raman processes, using generic level systems to describe them.
After the discussion of ionic solids we shift our attention to atomic vapours. Here, we discuss the dynamics of microscopic order within the angular momentum substates under the influence of light and magnetic fields. For this purpose, we combine optical pumping as outlined in Chapter 5 to prepare the ordered states, and polarisation-selective detection introduced in Chapter 6 for its observation. In contrast to the introductory sections, we no longer discuss these dynamics as mathematical models, but for specific physical systems, using experimental data to illustrate the theoretical description. The systems we use for this illustration are vapours of alkali metal atoms, in particular sodium. These one-electron systems allow the most direct application of the theoretical models developed above. In addition, we concentrate on electronic ground states, whose long lifetimes permit long observation times and correspondingly precise observations.
Experimental arrangement
General considerations
Laser-induced dynamics
This chapter surveys the coherent evolution of coherences between angular momentum sublevels. Optical pumping excites this microscopic order, and it evolves under the influence of external magnetic fields and the laser radiation. The primary goal of this section is to show how the mathematical models developed in the preceding sections apply to real physical systems. We discuss how the observed signals arise and by which parameters the experimenter can control the dynamics of these systems.
After the brief discussion of the internal degrees of freedom of atomic systems, we give an overview of how these variables can acquire nonvanishing average values in an ensemble of atoms. Optical pumping was one of the first experimental schemes that allowed physical systems to be pushed far from equilibrium through the interaction with light, a direct consequence of angular momentum conservation and the symmetry properties of the interaction between atoms and radiation.
Principle and overview
Phenomenology
Optical pumping (Happer 1972) is one of the earliest examples wherein optical radiation qualitatively modifies the properties of a material system. In its original implementation, it corresponds to a selective population of specific angular momentum states, starting from thermal equilibrium.
In the idealised process depicted in Figure 5.1, the light brings the atomic system from the initially disordered state, in which the populations of degenerate levels are equal, into an ordered state where the internal state of all atoms is the same. If we consider only the material system, it appears as if the evolution from the initially disordered state into an ordered state, where the population of one level is higher than that of another level, violated the second law of thermodynamics. This process does not proceed spontaneously, however. It is the interaction with polarised light that drives the system and increased disorder in the radiation field compensates for the increase in the population difference in the material system (Enk and Nienhuis 1992).
The two- and three-level model systems considered in the preceding sections can describe a wide range of phenomena. On the other hand, these models are purely mathematical constructs that lack physical content. The connection to physical systems is arbitrary and must be made separately in each case. In this chapter, we take the first step in this direction: We discuss the internal degrees of freedom that an atom has available. By far the most important ones are the electric dipole moment, which is responsible for the coupling to external fields, and the angular momentum, which determines the selection rules for the optical transitions and couples to magnetic fields.
Rotational symmetry
Motivation
The number of energy levels that contribute to the dynamics of a quantum mechanical system is a direct measure of the number of degrees of freedom required for a full description of the system. The systems in which we are interested always include electric dipole moments – the degrees of freedom that couple to the radiation field. The second most important contribution is the magnetic dipole moment associated with the atomic angular momentum. Electric and magnetic dipole moments are those degrees of freedom that couple to external fields. Other degrees of freedom do not couple strongly to external fields but they may still modify the behaviour of the system and its optical properties.
Two-dimensional spectroscopy is an extension of conventional spectroscopic methods that characterises resonant systems as a function of two frequency variables. We use this technique to improve on the characterisation of atomic media along the lines discussed in the preceding chapter. On a microscopic level, the most important physical process for two-dimensional spectroscopy is the transfer of coherence between different transitions. We introduce the basics of the technique and discuss a few specific examples to outline its potential.
Fundamentals
Motivation and principle
Motivation
The preceding chapter showed how light drives the internal dynamics of resonant atomic media and how the measurement of optical anisotropies allows us to monitor these dynamics. The experiments discussed in the preceding chapter, however, can provide only limited information about the system. Most physical systems have more degrees of freedom than we can observe by measurements on transmitted light. As another limitation, we have primarily considered atoms that evolve under their internal Hamiltonian, only weakly perturbed by the probe laser beam. The example of light-induced spin nutation showed that the dynamics of optically pumped atoms differ significantly from those of a free atom. Although it is possible to observe spin nutation for systems with more than two ground-state sublevels, such an experiment suffers from the damping that accompanies optical pumping. The damping drives the system rapidly to an equilibrium, too fast for detailed dynamical observations.
Light interacting with material substances is one of the prerequisites for life on our planet. More recently, it has become important for many technological applications, from CD players and optical communication to gravitational-wave astronomy. Physicists have therefore always tried to improve their understanding of the observed effects. The ultimate goal of such a development is always a microscopic description of the relevant processes. For a long time, this description was identical with a perturbation analysis of the material system in the external fields. More than a hundred years ago, such a microscopic theory was developed in terms of oscillating dipoles. After the development of quantum mechanics, these dipoles were replaced by quantum mechanical two-level systems, and this is still the most frequently used description.
However, the physical situation has changed qualitatively in the last decades. The development of intense, narrowband or pulsed lasers as tunable light sources has provided not only a new tool that allows much more detailed investigation, but also the observation of qualitatively new phenomena. These effects can no longer be analysed in the form of a perturbation expansion. One consequence is that the actual number of quantum mechanical states involved in the interaction becomes relevant. It is therefore not surprising that many newly discovered effects are associated with the details of the level structure of the medium used in the experiment. Two popular examples are the discovery of sub-Doppler laser cooling and the development of magnetooptical traps, which rely on the presence of angular momentum substates.
After the introduction of the two-level model, we add a third level to the quantum mechanical system to discuss some of the effects that cannot be described with only two states. The main feature is the exchange of order between states and transitions, which may proceed through populations or coherences. We concentrate our attention on the latter possibility.
Phenomenological introduction
Model atoms
In the preceding section, we discussed the interaction between light and two-level atoms – probably one of the most popular physical models. The basis of this popularity is its intuitively simple interpretation combined with the posibility of explaining a wide range of physical phenomena. An interesting aspect of the two-level system is that, although its dynamics are formally equivalent to those of a classical angular momentum, it can explain many aspects of quantum mechanics. Once these aspects are understood, it is tempting to look further into the behaviour of real systems, trying to find patterns inconsistent with the predictions of the two-level model.
This section discusses aspects of the interaction between matter and radiation that are incompatible with the two-level model. We do not consider specific atomic systems or attempt a complete analysis of the dynamics that a three-level system can exhibit. Instead we select a number of phenomena that play an important role in the discussion of those physical systems that form the subject of the subsequent sections.
Atomic physics is one of the oldest fields of physics. A barren and “academic” discipline? Not at all! About ten years ago, atomic physics received a rejuvenating jolt from chaos theory with far reaching implications. Chaos in atomic physics is today one of the most active and prolific areas in atomic physics. This book, addressed at interested students and practitioners alike, is a first attempt to provide a coherent introduction into this fascinating area of contemporary research. In line with its scope, the book is essentially divided into two parts. The first part of the book (Chapters 1 – 5) deals with the theory and philosophy of classical chaos. The ideas and concepts developed here are then applied to actual atomic and molecular physics systems in the second part of the book (Chapters 6 – 10).
When compiling the material for the first part of the book we profited immensely from a number of excellent tutorials on classical and quantum chaos. We mention the books by Lichtenberg and Lieberman (1983), Zaslavsky (1985), Schuster (1988), Sagdeev et al. (1988), Tabor (1989), Gutzwiller (1990), Haake (1991), Devaney (1992) and Reichl (1992).
The illustrative examples for the second part of the book were mostly taken from our own research work on the manifestations of chaos in atomic and molecular physics. We apologize at this point to all the numerous researchers whose work is not represented in this book. This has nothing to do with the quality of their work and is due only to the fact that we had to make a selection.
The stability of the solar system is one of the most important unsettled questions of classical mechanics. Even a simplified version of the solar system, the three-body problem, presents a formidable challenge. An important breakthrough occurred when Poincaré, with some assistance from his Swedish colleague Fragmen, proved in 1892 that, apart from some notable exceptions, the three-body problem does not possess a complete set of integrals of the motion. Thus, in modern parlance, the three-body problem is chaotic.
The helium atom is an atomic physics example of a three-body problem. On the basis of Poincaré's result we have to expect that the helium atom is classically chaotic. Richter and Wintgen (1990b) showed that this is indeed the case: the helium atom exhibits a mixed phase space with intermingled regular and chaotic regions (see also Wintgen et al. (1993)). Thus, conceptually, the helium atom is a close relative of the double pendulum studied in Section 3.2. Given the classical chaoticity of the helium atom we are confronted with an important question: How does chaos manifest itself in the helium atom?
In order to provide clues for an answer to this question we study in this chapter a one-dimensional version of the helium atom, the “stretched helium atom” (Watanabe (1987), Blümel and Reinhardt (1992)). This model, although only a “caricature” of the three-dimensional helium atom, is realistic enough to capture some of the most important physical features of the helium atom.
What happens if one sprinkles electrons onto the surface of liquid helium? Surprisingly the electrons are not absorbed into the bulk of the fluid, but form a quasi-two-dimensional sheet of electrons concentrated at some distance above the helium surface. In general, electrons hovering above the surface of a dielectric are called surface state electrons. An excellent review of surface state electrons is that by Cole (1974).
Surface state electrons are especially interesting in the context of chaos and quantum chaos. This is so because driven by strong microwave fields, their classical dynamics shows a transition to chaos. The investigation of microwave-driven surface state electrons as a testing ground for quantum chaos was first proposed by Jensen in 1982. So far, and to the best of our knowledge, a successful surface-state-electron (SSE) microwave ionization experiment was never carried out in the chaotic regime. This is mainly due to the formidable experimental difficulties in controlling the fragile SSE system. Electric stray fields, residual helium vapour pressure and interactions with the quantized surface modes (“ripplons”) of the liquid helium substrate make it very difficult to reach the high quantum numbers necessary for a quantum chaos experiment. It was, however, realized early on (see, e.g., Shepelyansky (1985)) that the dynamics of low angular momentum hydrogen Rydberg atoms is very similar to the dynamics of surface state electrons. Therefore, building on the knowledge accumulated in the field of surface state electrons, the focus of research shifted to the investigation of microwave-driven hydrogen and alkali Rydberg atoms.
Einstein (1917) appreciated early on that within the “old” pre-1925/26 quantum mechanics absence of integrability is a serious obstacle for the quantization of classical systems. Therefore, in retrospect not surprisingly, the quantization problem was not adequately solved until the advent of the “new” quantum mechanics by Heisenberg, Born, Jordan and Schrödinger. The new quantum mechanics did not rely at all on the notion of classical paths, and this way, unwittingly, sidestepped the chaos problem. Within the framework of the new theory, any classical system can be quantized, including classically chaotic systems. But while the quantization of integrable systems is straightforward, the quantization of classically chaotic systems, even today, presents a formidable technical challenge. This is especially true for quantization in the semiclassical regime, where the quantum numbers involved are large. In fact, efficient semiclassical quantization rules for chaotic systems were not known until Gutzwiller (1971, 1990) intoduced periodic orbit expansions. Gutzwiller's method is discussed in Section 4.1.3 below. It is important to emphasize here that the existence of chaos in certain classical systems in no way introduces conceptual problems into the framework of modern quantum theory, although, let it be emphasized again, chaos came back with a vengeance from the “old” days of quantum mechanics. Even given all the modern day computer power accessible to the “practitioner” of quantum mechanics, chaos is the ultimate reason for the slow progress in the numerical computation of even moderately excited states in such important, but chaotic problems as the helium atom.