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Journal of Mathematical Physics

A Model of Interacting Radiation and Matter

C. R. Willis

Published Sep 1, 1964• 26 citations
Publisher

Abstract

We investigate the long-time behavior of a model consisting of N two-level atoms in a lossless cavity. The Hamiltonian of our system contains the radiation oscillators in addition to the matter Hamiltonian and the usual ∫j·Adv interaction term. In order to treat the system perturbatively, it would be necessary to remove the tremendous degeneracy of the system. Since this is prohibitively difficult, and since we are interested in the long-time behavior of the system, we solve the quantum mechanical Liouville equation directly for a wide class of physically important initial distribution functions. We show the effective expansion parameter is γ̃Nγ̃ where γ̃ is a dimensionless atomic dipole moment and N is the number of atoms. In the lowest order we find the self-consistent field approximation. In the next order, particle-field correlations appear. We explicitly solve the equations of motion for the particle-field correlations in terms of the average quantities that appear in the self-consistent field approximation. We show the self-consistent field approximation consists of five first-order differential equations. Next we show the equations of motion for the density matrix of the system correct to order (γ̃Nγ̃)2 are equivalent to eight first-order differential equations. The three additional equations are needed to describe the three second moments of the density matrix of the electromagnetic field that appear in second order. Our lowest-order microscopic equations are equivalent to semiphenomenological theories and our higher-order equations contain only the measurable second-order moments of the electromagnetic field in addition to the variables that appear in semi-phenomenological theories.

DOI
10.1063/1.1704232

Related papers

A Model of Interacting Radiation and Matter. II

C. R. Willis

We extend the investigation of the long time behavior of a model consisting of N two-level atoms interacting with radiation to include dissipation, pumping, and center-of-mass motion. We show that when the effective expansion parameter γ̃Nγ̃ is small, the self-consistent field approximation remains the solution to lowest order in γ̃Nγ̃. The inclusion of the center-of-mass motion introduces another dimensionless parameter β into the theory. We show that when this parameter is small, the electromagnetic field amplitude varies slowly on the time scale of the center-of-mass motion. We solve the equations of motion in this slowly varying limit by an extension of the Bogoliuboff-Kryloff theory of quasilinearity to the problem of time-dependent integral kernals. We find the unique stable stationary state and show that in the slowly varying limit the stationary state is approached independent of initial conditions. We calculate the frequency shift to second order in β. The first-order frequency shift is the same as that calculated by Lamb. We compare our steady-state solution with recent experiments with lasers. We include the effect of collisions in the steady state.

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Self-fields in semiclassical radiation theory

Michael D. Crisp

The interaction of an atomic system with an unquantized electromagnetic field is studied by means of the Heisenberg-operator equations of motion. The electromagnetic fields created by the atom are taken into account by assuming that the charge and probability current densities are the actual charge and current source terms in Maxwell's equation. When Ehrenfest's theorem is written to order (1/c${)}^{2}$, the equations of motion are found to have a constant of motion that can be interpreted as stating that the sum of the atomic energy, energy of interaction, and energy stored in the electromagnetic field is constant. This constant of integration can be expressed as an expectation of a new semiclassical Hamiltonian that now includes the effects of the atomic self-fields to order 1/${\mathit{c}}^{2}$. This Hamiltonian is related to the classical Darwin Lagrangian. Since the new approximate Hamiltonian is the sum of an atomic and a field Hamiltonian, it provides a formulation of semiclassical radiation theory that is formally close to the usual formulation of quantum electrodynamics. A Schr\"odinger equation can be derived by applying the variational principle to the expectation of the new Hamiltonian. The result is a nonlinear integro-differential equation, in \ensuremath{\Psi}, which is somewhat similar to Hartree's self-consistent equation for a multielectron atom.When the Heisenberg equations are written to include the next-higher-order terms, 1/${\mathit{c}}^{3}$, it is found that the total energy of the atom and the electromagnetic field in the vicinity of the atom decreases at a rate that is given by the Larmor power formula (2${\mathit{e}}^{2}$/3${\mathit{c}}^{3}$)(d〈v〉/dt${)}^{2}$, where 〈v〉 is the quantum-mechanical expectation of the electron's velocity operator. This approximate formulation of semiclassical radiation theory is applied to semiclassical calculations of atomic radiative shifts. It is then shown that, if some retardation effects are included to all orders of 1/c in the vector potential, the semiclassical analysis provides a formula for radiative energy-level shifts that are time dependent and that contain coefficients similar to the starting point of the Bethe calculation of the Lamb shift. The incorporation of mass renormalization in semiclassical theory is then discussed.

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Based on the separability with respect to position variables of the susceptibility for a finite system, we have developed a formulation which solves Schri:idinger and Maxwell equations selfconsistently. The case of linear response is' described in detail. As a manifes­ tation of the selfconsistency between the two equations, the appearance of radiative damping rate with correct magnitude has been demonstrated for a two-level atom in vacuum. The interaction of electromagnetic (EM) radiation with matter has been studied in various aspects for quite a long time. The relevant phenomena range, in the scale of wavelength, from rf wave (NMR, for example) to gamma ray (Mossbauer effect): They are related with the absorption, reflection, transmission, propagation, refrac­ tion, scattering, diffraction, emission, etc. of EM wave in linear and nonlinear manner. For the theoretical treatment of these phenomena, we need Schrodinger equation for the description of matter and Maxwell equations in classical or quantized form for radiation field. When the Maxwell equations are treated in classical form, this is called semiclassical treatment of radiation-matter interaction. Though it has a certain limitation, the semiclassical treatment can be appliedto most of the phenom­ ena mentioned above. For the treatment of the interaction of EM radiation with solids, it is usual to employ a susceptibility function to describe the solid, and solve the Maxwell equa­ tions containing that susceptibility as an integral kernel. In doing so, we must consider the boundary conditions (BC) arising from the shape of the sample in question. However, we do not consider BC's in treating microscopic systems such as an atom or small molecule. This would mean that the use of BC(s is in general not compulsory, although we are so much accustomed to it. In this respect, there has been a long debated problem of additional boundary condition (ABC) in relation with exciton polaritons in semiconductors or insulators, where the nonlocal nature of the medium allows the existence of two or more eigenmodes of the coupled exciton-EM radiation. After the long history of the ABC problem,r>- 4 > we now have a recipe to derive the appropriate form(s) of ABC(s) from a microscopic model of the medium including the details of the surface. 5 >-s> Another form of the microscopic solution of the ABC problem has been given as an ABC-free formulation, 9 >-n> where one needs

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Coherence in a Model of Interacting Radiation and Matter

Richard H. Picard, C. R. Willis

Some preliminary results of a theoretical investigation of the origin of laser coherence properties are presented. A model consisting of $N$ two-level atoms in a perfect cavity interacting through their dipole moments with a single mode of the radiation field is adopted, and the resulting many-body problem is made solvable through the introduction of the self-consistent-field approximation (SCFA). It is shown that the SCFA is consistent with Glauber's suggestion that an ideal laser might be in a "coherent state," or pure eigenstate of the positive-frequency part of the electric-field operator. A conservation law is derived which assures the positive definiteness of the field-density operator, and it is shown that Glauber's coherent state is that solution of the SCFA equations which minimizes the corresponding constant of the motion. When the SCFA is modified by the introduction of particle-field correlations, the conservation law is destroyed, and the coherent state is no longer and allowed solution.

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Coupled Superradiance Master Equations

Richard H. Picard, C. R. Willis

In this paper we attempt to unify the theoretical treatment of a variety of cooperative interaction phenomena occurring in resonantly interacting radiation-matter systems. The system consists of a multimode optical field interacting with $N$ resonant atoms in a region of large spatial extent. The field and atoms may or may not be coupled to reservoirs. We derive a set of coupled master equations for the reduced matter and radiation density operators of the composite system in the first Born approximation, using a method due to Bogoliubov. These equations describe within a single framework phenomena involving superradiant emission and coherent propagation. In the first place, our theory generalizes existing formulations of the superradiance problem by treating the radiation field as part of the dynamical system rather than as a reservoir. Hence, our equations describe stimulated interaction effects, which are entirely absent in the usual superradiance master equations. Moreover, our equations contain terms describing the self-consistent interaction of an average field with a set of polarizable atoms, as in the coupled Bloch and Maxwell equations of the theory of coherent pulse propagation, and enable us to describe fluctuations, arising from incoherent emission, about the average behavior described by the Bloch-Maxwell theory. We solve formally the dynamical equation for the radiation density operator and obtain a displaced multivariate Gaussian distribution centered on the solution of the Maxwell wave equation, which has as parameters the first and second moments of the matter density operator. Then we derive and discuss the field and atomic-moment equations, both in the wave-number and position representations. The moment equations enable us to show the relationship between descriptions of superradiant damping based on the Bloch equations and those based on the existence of correlated atomic states, including both as special cases. We introduce reduced matter moments, which allow us to separate incoherent- and coherent-emission effects and enable us to discuss the question of the closure of the moment equations. Then we consider cases where the behavior of the atomic system is dominated by a strong coherent pump wave or where the atoms are in a symmetric correlated state and show how the slowly-varying-envelope approximation simplifies the radiation-moment equations in these two cases. In the former case, we obtain an approximate theory which consists, in lowest order, of the Bloch-Maxwell equations with radiative-damping terms, plus an equation describing the time development of the correlation function for field fluctuations. Returning to our general formalism, we relate the usual parameters of the theory of radiative decay and of resonant interactions to the more general quantities appearing in our spatial analysis. Finally, we discuss the importance of the stimulated-emission terms appearing in our theory and describe several extensions, including the introduction of inhomogeneous broadening.

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Quantum theory of radiation

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Atoms and ions containing residual bound electrons do not quite resemble the simple harmonic oscillator model used so successfully in the classical theory of radiation. However, replacing the atoms or ions with sets of harmonic oscillators of a great number of discrete resonance frequencies and having various amplitudes, together with the results of classical radiation theory, go a long way toward a quantitative description of emission or absorption spectra. The set of resonance frequencies is obtained from measured or calculated energy levels using Ritz's combination principle. The amplitudes are associated with matrix elements of appropriate quantum mechanical operators between wave functions of the two energy eigenstates involved at a given frequency. In other words, quantities of the emitters, absorbers, or scatterers are described quantum-mechanically, whereas the electromagnetic field is treated classically. Such semi-classical description of matter-electromagnetic field interactions became unnecessary very early in the development of quantum theory. It will therefore not be discussed in any detail. Instead, we will begin immediately with the combined theory of matter and radiation (Heitler 1954, Dirac 1958, Loudon 1983). Quantum theory of particles and fields There are various ways to also quantize the electromagnetic fields (Cohen-Tannoudji, DuPont-Roc and Grynberg 1989), of which that performed on the combined Hamiltonian equations of motion for the field-matter system is followed here.

Cambridge University Press eBooks•Oct 2, 1997•19 citations
We investigate the long-time behavior of a model consisting of N two-level atoms in a lossless cavity. The Hamiltonian of our system contains the radiation oscillators in addition to the matter Hamiltonian and the usual ∫j·Adv interaction term. In order to treat the system perturbatively, it would be necessary to remove the tremendous degeneracy of the system. Since this is prohibitively difficult, and since we are interested in the long-time behavior of the system, we solve the quantum mechanical Liouville equation directly for a wide class of physically important initial distribution functions. We show the effective expansion parameter is γ̃Nγ̃ where γ̃ is a dimensionless atomic dipole moment and N is the number of atoms. In the lowest order we find the self-consistent field approximation. In the next order, particle-field correlations appear. We explicitly solve the equations of motion for the particle-field correlations in terms of the average quantities that appear in the self-consistent field approximation. We show the self-consistent field approximation consists of five first-order differential equations. Next we show the equations of motion for the density matrix of the system correct to order (γ̃Nγ̃)2 are equivalent to eight first-order differential equations. The three additional equations are needed to describe the three second moments of the density matrix of the electromagnetic field that appear in second order. Our lowest-order microscopic equations are equivalent to semiphenomenological theories and our higher-order equations contain only the measurable second-order moments of the electromagnetic field in addition to the variables that appear in semi-phenomenological theories.
We extend the investigation of the long time behavior of a model consisting of N two-level atoms interacting with radiation to include dissipation, pumping, and center-of-mass motion. We show that when the effective expansion parameter γ̃Nγ̃ is small, the self-consistent field approximation remains the solution to lowest order in γ̃Nγ̃. The inclusion of the center-of-mass motion introduces another dimensionless parameter β into the theory. We show that when this parameter is small, the electromagnetic field amplitude varies slowly on the time scale of the center-of-mass motion. We solve the equations of motion in this slowly varying limit by an extension of the Bogoliuboff-Kryloff theory of quasilinearity to the problem of time-dependent integral kernals. We find the unique stable stationary state and show that in the slowly varying limit the stationary state is approached independent of initial conditions. We calculate the frequency shift to second order in β. The first-order frequency shift is the same as that calculated by Lamb. We compare our steady-state solution with recent experiments with lasers. We include the effect of collisions in the steady state.
The interaction of an atomic system with an unquantized electromagnetic field is studied by means of the Heisenberg-operator equations of motion. The electromagnetic fields created by the atom are taken into account by assuming that the charge and probability current densities are the actual charge and current source terms in Maxwell's equation. When Ehrenfest's theorem is written to order (1/c)2{)}^{2})2, the equations of motion are found to have a constant of motion that can be interpreted as stating that the sum of the atomic energy, energy of interaction, and energy stored in the electromagnetic field is constant. This constant of integration can be expressed as an expectation of a new semiclassical Hamiltonian that now includes the effects of the atomic self-fields to order 1/c2{\mathit{c}}^{2}c2. This Hamiltonian is related to the classical Darwin Lagrangian. Since the new approximate Hamiltonian is the sum of an atomic and a field Hamiltonian, it provides a formulation of semiclassical radiation theory that is formally close to the usual formulation of quantum electrodynamics. A Schr\"odinger equation can be derived by applying the variational principle to the expectation of the new Hamiltonian. The result is a nonlinear integro-differential equation, in \ensuremath{\Psi}, which is somewhat similar to Hartree's self-consistent equation for a multielectron atom.When the Heisenberg equations are written to include the next-higher-order terms, 1/c3{\mathit{c}}^{3}c3, it is found that the total energy of the atom and the electromagnetic field in the vicinity of the atom decreases at a rate that is given by the Larmor power formula (2e2{\mathit{e}}^{2}e2/3c3{\mathit{c}}^{3}c3)(d〈v〉/dt)2{)}^{2})2, where 〈v〉 is the quantum-mechanical expectation of the electron's velocity operator. This approximate formulation of semiclassical radiation theory is applied to semiclassical calculations of atomic radiative shifts. It is then shown that, if some retardation effects are included to all orders of 1/c in the vector potential, the semiclassical analysis provides a formula for radiative energy-level shifts that are time dependent and that contain coefficients similar to the starting point of the Bethe calculation of the Lamb shift. The incorporation of mass renormalization in semiclassical theory is then discussed.
Based on the separability with respect to position variables of the susceptibility for a finite system, we have developed a formulation which solves Schri:idinger and Maxwell equations selfconsistently. The case of linear response is' described in detail. As a manifes­ tation of the selfconsistency between the two equations, the appearance of radiative damping rate with correct magnitude has been demonstrated for a two-level atom in vacuum. The interaction of electromagnetic (EM) radiation with matter has been studied in various aspects for quite a long time. The relevant phenomena range, in the scale of wavelength, from rf wave (NMR, for example) to gamma ray (Mossbauer effect): They are related with the absorption, reflection, transmission, propagation, refrac­ tion, scattering, diffraction, emission, etc. of EM wave in linear and nonlinear manner. For the theoretical treatment of these phenomena, we need Schrodinger equation for the description of matter and Maxwell equations in classical or quantized form for radiation field. When the Maxwell equations are treated in classical form, this is called semiclassical treatment of radiation-matter interaction. Though it has a certain limitation, the semiclassical treatment can be appliedto most of the phenom­ ena mentioned above. For the treatment of the interaction of EM radiation with solids, it is usual to employ a susceptibility function to describe the solid, and solve the Maxwell equa­ tions containing that susceptibility as an integral kernel. In doing so, we must consider the boundary conditions (BC) arising from the shape of the sample in question. However, we do not consider BC's in treating microscopic systems such as an atom or small molecule. This would mean that the use of BC(s is in general not compulsory, although we are so much accustomed to it. In this respect, there has been a long debated problem of additional boundary condition (ABC) in relation with exciton polaritons in semiconductors or insulators, where the nonlocal nature of the medium allows the existence of two or more eigenmodes of the coupled exciton-EM radiation. After the long history of the ABC problem,r>- 4 > we now have a recipe to derive the appropriate form(s) of ABC(s) from a microscopic model of the medium including the details of the surface. 5 >-s> Another form of the microscopic solution of the ABC problem has been given as an ABC-free formulation, 9 >-n> where one needs
Some preliminary results of a theoretical investigation of the origin of laser coherence properties are presented. A model consisting of NNN two-level atoms in a perfect cavity interacting through their dipole moments with a single mode of the radiation field is adopted, and the resulting many-body problem is made solvable through the introduction of the self-consistent-field approximation (SCFA). It is shown that the SCFA is consistent with Glauber's suggestion that an ideal laser might be in a "coherent state," or pure eigenstate of the positive-frequency part of the electric-field operator. A conservation law is derived which assures the positive definiteness of the field-density operator, and it is shown that Glauber's coherent state is that solution of the SCFA equations which minimizes the corresponding constant of the motion. When the SCFA is modified by the introduction of particle-field correlations, the conservation law is destroyed, and the coherent state is no longer and allowed solution.
In this paper we attempt to unify the theoretical treatment of a variety of cooperative interaction phenomena occurring in resonantly interacting radiation-matter systems. The system consists of a multimode optical field interacting with NNN resonant atoms in a region of large spatial extent. The field and atoms may or may not be coupled to reservoirs. We derive a set of coupled master equations for the reduced matter and radiation density operators of the composite system in the first Born approximation, using a method due to Bogoliubov. These equations describe within a single framework phenomena involving superradiant emission and coherent propagation. In the first place, our theory generalizes existing formulations of the superradiance problem by treating the radiation field as part of the dynamical system rather than as a reservoir. Hence, our equations describe stimulated interaction effects, which are entirely absent in the usual superradiance master equations. Moreover, our equations contain terms describing the self-consistent interaction of an average field with a set of polarizable atoms, as in the coupled Bloch and Maxwell equations of the theory of coherent pulse propagation, and enable us to describe fluctuations, arising from incoherent emission, about the average behavior described by the Bloch-Maxwell theory. We solve formally the dynamical equation for the radiation density operator and obtain a displaced multivariate Gaussian distribution centered on the solution of the Maxwell wave equation, which has as parameters the first and second moments of the matter density operator. Then we derive and discuss the field and atomic-moment equations, both in the wave-number and position representations. The moment equations enable us to show the relationship between descriptions of superradiant damping based on the Bloch equations and those based on the existence of correlated atomic states, including both as special cases. We introduce reduced matter moments, which allow us to separate incoherent- and coherent-emission effects and enable us to discuss the question of the closure of the moment equations. Then we consider cases where the behavior of the atomic system is dominated by a strong coherent pump wave or where the atoms are in a symmetric correlated state and show how the slowly-varying-envelope approximation simplifies the radiation-moment equations in these two cases. In the former case, we obtain an approximate theory which consists, in lowest order, of the Bloch-Maxwell equations with radiative-damping terms, plus an equation describing the time development of the correlation function for field fluctuations. Returning to our general formalism, we relate the usual parameters of the theory of radiative decay and of resonant interactions to the more general quantities appearing in our spatial analysis. Finally, we discuss the importance of the stimulated-emission terms appearing in our theory and describe several extensions, including the introduction of inhomogeneous broadening.
Atoms and ions containing residual bound electrons do not quite resemble the simple harmonic oscillator model used so successfully in the classical theory of radiation. However, replacing the atoms or ions with sets of harmonic oscillators of a great number of discrete resonance frequencies and having various amplitudes, together with the results of classical radiation theory, go a long way toward a quantitative description of emission or absorption spectra. The set of resonance frequencies is obtained from measured or calculated energy levels using Ritz's combination principle. The amplitudes are associated with matrix elements of appropriate quantum mechanical operators between wave functions of the two energy eigenstates involved at a given frequency. In other words, quantities of the emitters, absorbers, or scatterers are described quantum-mechanically, whereas the electromagnetic field is treated classically. Such semi-classical description of matter-electromagnetic field interactions became unnecessary very early in the development of quantum theory. It will therefore not be discussed in any detail. Instead, we will begin immediately with the combined theory of matter and radiation (Heitler 1954, Dirac 1958, Loudon 1983). Quantum theory of particles and fields There are various ways to also quantize the electromagnetic fields (Cohen-Tannoudji, DuPont-Roc and Grynberg 1989), of which that performed on the combined Hamiltonian equations of motion for the field-matter system is followed here.