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The Journal of Chemical Physics

Quantum dynamics of a molecule (atom) in a coherent radiation field

Karl F. Freed, A. A. Villaeys

Published Mar 15, 1979• 8 citations
Publisher

Abstract

We consider the description of the quantum dynamics of a two-level system interacting with a single Glauber coherent mode of the radiation field. An exact solution (within the rotating wave and electric dipole approximations) is provided for both the time-independent and time-dependent Green’s functions for the coupled matter–radiation system. The atom (molecular) transition probabilities are shown to be Poisson averages of the corresponding semiclassical problem when the latter is likewise treated in the rotating wave approximation. At low radiation intensities, the quantum and semiclassical results differ, but at high intensities, they become the same when the average photon number n0 in the field satisfies the condition n01/2≫1. A similar behavior is displayed for the expectation value of the electric field of the coherent mode in the presence of the atom. The spectrum of the radiation, resonantly scattered by the atom, is shown to coincide with the results of Mollow.

DOI
10.1063/1.437792

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Physical Review A•Dec 1, 1986•11 citations
We consider the description of the quantum dynamics of a two-level system interacting with a single Glauber coherent mode of the radiation field. An exact solution (within the rotating wave and electric dipole approximations) is provided for both the time-independent and time-dependent Green’s functions for the coupled matter–radiation system. The atom (molecular) transition probabilities are shown to be Poisson averages of the corresponding semiclassical problem when the latter is likewise treated in the rotating wave approximation. At low radiation intensities, the quantum and semiclassical results differ, but at high intensities, they become the same when the average photon number n0 in the field satisfies the condition n01/2≫1. A similar behavior is displayed for the expectation value of the electric field of the coherent mode in the presence of the atom. The spectrum of the radiation, resonantly scattered by the atom, is shown to coincide with the results of Mollow.
We introduce a combination of coherent states as variational test functions for the atomic and radiation sectors to describe a system of N a three-level atoms interacting with a one-mode quantised electromagnetic field, with and without the rotating wave approximation, which preserves the symmetry presented by the Hamiltonian. These provide us with the possibility of finding analytical solutions for the ground and first excited states. We study the properties of these solutions for the V -configuration in the double resonance condition, and calculate the expectation values of the number of photons, the atomic populations, the total number of excitations, and their corresponding fluctuations. We also calculate the photon number distribution and the linear entropy of the reduced density matrix to estimate the entanglement between matter and radiation. For the first time, we exhibit analytical expressions for all of these quantities, as well as an analytical description for the phase diagram in parameter space, which distinguishes the normal and collective regions, and which gives us all the quantum phase transitions of the ground state from one region to the other as we vary the interaction parameters (the matter-field coupling constants) of the model, in functional form.
In the preceding chapters concerning the interaction of a radiation field with matter, we assumed the field to be classical. In many situations this assumption is valid. There are, however, many instances where a classical field fails to explain experimentally observed results and a quantized description of the field is required. This is, for example, true of spontaneous emission in an atomic system which was described phenomenologically in Chapter 5. For a rigorous treatment of the atomic level decay in free space, we need to consider the interaction of the atom with the vacuum modes of the universe. Even in the simplest system involving the interaction of a single-mode radiation field with a single two-level atom, the predictions for the dynamics of the atom are quite different in the semiclassical theory and the fully quantum theory. In the absence of the decay process, the semiclassical theory predicts Rabi oscillations for the atomic inversion whereas the quantum theory predicts certain collapse and revival phenomena due to the quantum aspects of the field. These interesting quantum field theoretical predictions have been experimentally verified. In this chapter we discuss the interaction of the quantized radiation field with the two-level atomic system described by a Hamiltonian in the dipole and the rotating-wave approximations. For a single-mode field it reduces to a particularly simple form. This is a very interesting Hamiltonian in quantum optics for several reasons. First, it can be solved exactly for arbitrary coupling constants and exhibits some true quantum dynamical effects such as collapse followed by periodic revivals of the atomic inversion.
The problem of a single two level atom in its excited state, placed in a cavity in which no photons are present initially, and interacting with N modes of the electromagnetic field is solved exactly in the electric dipole, rotating wave approximation. Expressions for the energy eigenvalues and eigenvectors are derived, and an exact representation for the time dependent wavefunction of the system is given. These quantities are evaluated analytically for N=1,2 and 3, and the time dependent properties of the system for these values of N are investigated and discussed.
We compare the semiclassical and quantum predictions for the unitary dynamics of a two-level atom interacting with a single-mode electromagnetic field under parametric modulation of the atomic parameters in the regime of multiphoton atom–field resonances. We derive approximate analytic solutions for the semiclassical Rabi model when the atomic transition frequency and the atom–field coupling strength undergo harmonic external modulations. These solutions are compared to the predictions of the quantum Rabi model, which we solve numerically for an initial coherent state with a large average photon number (on the order of 104), in the regime of three-photon resonance. We show that, for short enough times and sufficiently intense coherent states, the semiclassical dynamics agrees quite well with the quantum dynamics, although it inevitably fails at longer times due to the absence of collapse–revival behavior. Furthermore, we describe how the field state evolves throughout the interaction, presenting numerical results for the average photon number, entropies (related to atom–field entanglement), and other quantities characterizing the photon number statistics of the electromagnetic field.
The interaction between a coherently oscillating radiation field, such as is generally encountered in micro-wave experiments, and a number of similar atomic systems coupled to the field through their electric dipole moments is analyzed for the case of resonance between atomic system and field, with both the field and molecules treated quantum-mechanically. Expressions are derived for the expectation value of field strength and the energy, and comparison between the two makes it possible to distinguish between coherent and incoherent parts of the energy, the former having its counterpart in the expectation value of the field strength, while the latter has no such counterpart. Terms corresponding to induced and spontaneous emission are identified, and it is shown that the latter includes both coherent and incoherent components. Special situations related to masers and to the coherence of spontaneous radiation are discussed. The distinction between the behavior of correlated and uncorrelated states is examined, and it is shown that both the coherent emission from uncorrelated states and the incoherent emission from correlated states may be proportional to the square of the number of molecules. The phase of the field is predictable for the coherent emission but unpredictable for the incoherent emission.
A model of a coupled atom---quantum-field system is presented, consisting of a time-independent Hamiltonian and a realistic dynamical initial condition. The Hamiltonian describes a fixed bound atom coupled to the complete electromagnetic field. The initial condition is a consistent quantum-mechanical description of an atom in the exact ground state of the coupled atom-field system, on which is superimposed an approaching quasiclassical excitation of the field which will cause the interesting dynamical processes later on. Tools are presented for the manipulation of this model, with emphasis towards series expansions of all relevant quantities suitable for small strength $\ensuremath{\lambda}$ of the atom-field coupling and (potentially) large magnitude $\ensuremath{\alpha}$ of the coherent field excitation, such that the "influence of the coherent excitation on the atom" (i.e., the product $\ensuremath{\lambda}\ensuremath{\alpha}$) remains constant as $\ensuremath{\lambda}$ tends to zero. The following results are obtained, at the lowest nontrivial order in $\ensuremath{\lambda}$, in an approximation suitable for times much shorter than any radiative lifetime of the atom: (a) The change in free-field energy due to the interaction with the atom is exactly compensated at all times by the change in bare-atom energy plus the atom-field coupling energy. This checks the consistency of the proposed scheme. (b) The frequency distribution of this change in free-field energy has a (somewhat unexpected) component, with a smooth spectrum, spreading over the whole width of the spectrum of the exciting pulse, in addition to $\ensuremath{\delta}$ and dispersive singularities centered on the atomic transition frequencies. This frequency distribution is discussed in detail and its features are illustrated by a number of figures, in a simple case, numerically tractable. (c) The heterodyne detection of the radiation emitted by the atom is investigated, with emphasis on the issue of causality and propagation of light. Strict causality is obtained, without further approximation, in a model with an atom-field coupling involving the field at a single point and a detector similarly sensitive to properties of the field at a single point. This result breaks down if one uses nonlocal approximations such as the rotating-wave approximation or a detection observable ${\mathbf{E}}^{\ensuremath{-}}(\mathbf{r})\ifmmode\cdot\else\textperiodcentered\fi{}{\mathbf{E}}^{+}(\mathbf{r})$. Finally, an appendix is devoted to the use, in quantum mechanics, of bases moving with respect to each other.